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  <front>
    <journal-meta><journal-id journal-id-type="publisher">SOIL</journal-id><journal-title-group>
    <journal-title>SOIL</journal-title>
    <abbrev-journal-title abbrev-type="publisher">SOIL</abbrev-journal-title><abbrev-journal-title abbrev-type="nlm-ta">SOIL</abbrev-journal-title>
  </journal-title-group><issn pub-type="epub">2199-398X</issn><publisher>
    <publisher-name>Copernicus Publications</publisher-name>
    <publisher-loc>Göttingen, Germany</publisher-loc>
  </publisher></journal-meta>
    <article-meta>
      <article-id pub-id-type="doi">10.5194/soil-9-479-2023</article-id><title-group><article-title>Research and management challenges following soil and landscape
decontamination at the onset of the reopening of the Difficult-to-Return
Zone, Fukushima (Japan)</article-title><alt-title>Research and management challenges following soil and landscape
decontamination</alt-title>
      </title-group><?xmltex \runningtitle{Research and management challenges following soil and landscape
decontamination}?><?xmltex \runningauthor{O.~Evrard et al.}?>
      <contrib-group>
        <contrib contrib-type="author" corresp="yes" rid="aff1">
          <name><surname>Evrard</surname><given-names>Olivier</given-names></name>
          <email>olivier.evrard@lsce.ipsl.fr</email>
        <ext-link>https://orcid.org/0000-0002-3503-6543</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff1">
          <name><surname>Chalaux-Clergue</surname><given-names>Thomas</given-names></name>
          
        <ext-link>https://orcid.org/0000-0003-3525-832X</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff2 aff3">
          <name><surname>Chaboche</surname><given-names>Pierre-Alexis</given-names></name>
          
        </contrib>
        <contrib contrib-type="author" corresp="no" rid="aff3">
          <name><surname>Wakiyama</surname><given-names>Yoshifumi</given-names></name>
          
        <ext-link>https://orcid.org/0000-0001-6085-7063</ext-link></contrib>
        <contrib contrib-type="author" corresp="no" rid="aff4">
          <name><surname>Thiry</surname><given-names>Yves</given-names></name>
          
        </contrib>
        <aff id="aff1"><label>1</label><institution>Laboratoire des Sciences du Climat et de l'Environnement
(LSCE/IPSL), Université Paris-Saclay,<?xmltex \hack{\break}?> UMR 8212 (CEA-CNRS-UVSQ),
Gif-sur-Yvette, France</institution>
        </aff>
        <aff id="aff2"><label>2</label><institution>International Research Fellow of Japan Society for the Promotion of
Science (Postdoctoral Fellowships for Research in Japan (Standard), Japan</institution>
        </aff>
        <aff id="aff3"><label>3</label><institution>Institute of Environmental Radioactivity, Fukushima University, Kanayagawa, Japan</institution>
        </aff>
        <aff id="aff4"><label>4</label><institution>French National Radioactive Waste Management Agency (Andra) –<?xmltex \hack{\break}?>
Research and Development Division, Bure, France</institution>
        </aff>
      </contrib-group>
      <author-notes><corresp id="corr1">Olivier Evrard (olivier.evrard@lsce.ipsl.fr)</corresp></author-notes><pub-date><day>6</day><month>September</month><year>2023</year></pub-date>
      
      <volume>9</volume>
      <issue>2</issue>
      <fpage>479</fpage><lpage>497</lpage>
      <history>
        <date date-type="received"><day>14</day><month>April</month><year>2023</year></date>
           <date date-type="rev-request"><day>8</day><month>May</month><year>2023</year></date>
           <date date-type="rev-recd"><day>4</day><month>July</month><year>2023</year></date>
           <date date-type="accepted"><day>2</day><month>August</month><year>2023</year></date>
      </history>
      <permissions>
        <copyright-statement>Copyright: © 2023 Olivier Evrard et al.</copyright-statement>
        <copyright-year>2023</copyright-year>
      <license license-type="open-access"><license-p>This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit <ext-link ext-link-type="uri" xlink:href="https://creativecommons.org/licenses/by/4.0/">https://creativecommons.org/licenses/by/4.0/</ext-link></license-p></license></permissions><self-uri xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023.html">This article is available from https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023.html</self-uri><self-uri xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023.pdf">The full text article is available as a PDF file from https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023.pdf</self-uri>
      <abstract><title>Abstract</title>

      <p id="d1e142">Twelve years after the nuclear accident that occurred at the
Fukushima Dai-ichi Nuclear Power Plant (FDNPP) in March 2011, radiocesium
contamination (with a large dominance of <inline-formula><mml:math id="M1" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs, with a 30-year
half-life) remains a major concern in various municipalities of north-eastern
Japan. The Japanese authorities completed an unprecedented soil
decontamination programme in residential and cultivated areas affected by
the main radioactive plume (8953 km<inline-formula><mml:math id="M2" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>). They implemented a
complex remediation programme scheme to remediate soils that are fundamental
to life on Earth, relying on different decision rules depending on the waste
type, its contamination level and its region of origin, after delineating
different zones exposed to contrasted radiation rates. The central objective
was not to expose local inhabitants to radioactive doses exceeding 1 mSv yr<inline-formula><mml:math id="M3" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in addition to the natural levels. At the onset of the full
reopening of the Difficult-to-Return Zone (DTRZ) in spring 2023, the current review
provides an update of a previous synthesis published in 2019
(Evrard et al., 2019). Although this ambitious soil remediation
and reconstruction programme has almost been completed in the 12 municipalities
of Fukushima Prefecture in which an evacuation order was imposed in at least
one neighbourhood in 2011, from the 147 443 inhabitants who lived there
before the accident, only 29.9 % of them had returned by 2020. Waste
generated by decontamination and tsunami cleaning/demolition work is planned
to have been fully transported to (interim) storage facilities by the end of
2023. The cost of the operations conducted between 2011 and 2020 for the
so-called “nuclear recovery” operations (including decontamination) was
estimated by the Board of Audit of Japan in 2023 as JPY 6122.3 billion
(<inline-formula><mml:math id="M4" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> EUR 44 billion). Decontamination of cropland was shown to
have impacted soil fertility, and potassium fertilisation is recommended to
limit the transfer of residual radiocesium to new crops. In forests that
cover 71 % of the surface area of Fukushima Prefecture and that were
not targeted by remediation, radiocesium is now found in the upper mineral
layer of the soil in a quasi-equilibrium state. Nevertheless, <inline-formula><mml:math id="M5" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations in forest products (including wood for heating and
construction, wild plants, wildlife game, mushrooms) often keep exceeding
the threshold values authorised in Japan, which prohibits their exploitation
in the area affected by the main plume. Radionuclides from forests were shown
to be exported in dissolved and particle-bound forms to downstream river
systems and floodplains, although multiple monitoring records showed the
continuous decrease in radiocesium concentrations in both river water and
sediment across the main plume between 2011 and 2021. Fish contamination is now
generally found to be below the threshold limits although reputational damage
remains a major concern for local fishing communities. The remobilisation<?pagebreak page480?> of
radiocesium from sediment accumulated in reservoirs of the region is also of
potential concern as it may lead to secondary contamination of fish or
irrigation waters supplied to decontaminated fields. Overall, this synthesis
demonstrates the need to continue monitoring post-accidental radiocesium
transfer in these environments and to keep sharing data in order to refine
our predictive understanding of radiocesium mobility and consolidate the
tools available to model contaminant transfer in ecosystems. In forests in
particular, novel countermeasures and wood uses remain to be developed and
tested. Furthermore, the hydrologic connectivity between soils under
different ecosystems greatly influences long-term radiocesium
transport. The consequences of extreme phenomena (e.g. typhoons, forest
fires) that may become more frequent in the future as a result of global
change in these contaminated environments should be further anticipated.</p>
  </abstract>
    </article-meta>
  </front>
<body>
      

<sec id="Ch1.S1" sec-type="intro">
  <label>1</label><title>Introduction</title>
      <p id="d1e200">The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident that occurred in
March 2011 resulted in the emissions of large quantities of radionuclides
into the environment (Morino et al., 2013). Among these
radionuclides, more than 10 years after the accident, radiocesium is the
most problematic substance (mainly for its longer-lived <inline-formula><mml:math id="M6" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs isotope
(<inline-formula><mml:math id="M7" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">30</mml:mn></mml:mrow></mml:math></inline-formula> years) as less than 10 % of the shorter-lived
<inline-formula><mml:math id="M8" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">134</mml:mn></mml:msup></mml:math></inline-formula>Cs isotope (<inline-formula><mml:math id="M9" display="inline"><mml:mrow><mml:msub><mml:mi>T</mml:mi><mml:mrow><mml:mn mathvariant="normal">1</mml:mn><mml:mo>/</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msub><mml:mo>=</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:math></inline-formula> years) emitted initially in similar
quantities as <inline-formula><mml:math id="M10" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs was still found in the environment by 2022). The
fraction of other isotopes such as those of plutonium that was supplied by
the FDNPP accident and that were detected shortly after March 2011 in
environmental samples (2011–2013) have no been longer detected in the last
years (Diacre et al., 2023). As the main radioisotope being found in the
vicinity of FDNPP 12 years after the accident, <inline-formula><mml:math id="M11" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs is a gamma
emitter that is quickly bound to clay minerals (mainly micas such as illite
and vermiculite), which show frayed-edge sites with high selectivity for
Cs<inline-formula><mml:math id="M12" display="inline"><mml:msup><mml:mi/><mml:mo>+</mml:mo></mml:msup></mml:math></inline-formula> cations (Cremers et al., 1988; Okumura et al., 2018).
Accordingly, <inline-formula><mml:math id="M13" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs may therefore persist in soils and contaminate them
for several decades, which may prevent them from fulfilling their functions and providing the expected ecosystem services (Keesstra et al., 2016).
Possible exposure of organisms to radiations emitted by radiocesium found in
soils and other environmental compartments together with the food chain
contamination justified the evacuation and/or the decontamination of those
zones exposed to radiation dose rates exceeding a given threshold – i.e.
typically 20 mSv yr<inline-formula><mml:math id="M14" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in emergency conditions and 1 mSv yr<inline-formula><mml:math id="M15" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in
“normal” conditions as recommended by the International Commission on Radiological Protection (ICRP, 2020; Lyons et al., 2020). Although the impact of high radiation doses is debated for Fukushima,
a recent study showed the natural rewilding of the Fukushima landscape
following human abandonment, and suggested that if any effects of
radiological exposure in mid- to large-sized mammals in the Fukushima
Exclusion Zone existed, they occurred at individual or molecular scales, and
did not appear to manifest (or have not yet manifested) in population-level
responses (Lyons et al., 2020). Another potential issue associated with
<inline-formula><mml:math id="M16" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs is related to the fact that different types of microparticles
bearing this radioisotope were found in the environment and that their
inhalation may lead to specific health risks (Hagiwara et al.,
2021; Okumura et al., 2019; Miura et al., 2018).</p>
      <p id="d1e331">Contrary to the situation observed after the Chernobyl accident, where a
large (i.e. 30 km radius zone) contaminated area remained evacuated and
abandoned for several decades, resulting in a large-scale rewilding of the
area (Fesenko et al., 2022), the Japanese authorities decided
to conduct ambitious decontamination works in residential and cultivated
areas affected by the main radioactive plume
(Yasutaka and Naito, 2016). Different zones were
delineated to organise decontamination works depending on the initial
radioactive contamination levels found in these zones and the resulting
exposition of inhabitants and workers to radiation dose rates. The long-term
goal was to keep individual exposure doses below 1 mSv yr<inline-formula><mml:math id="M17" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> or 0.23 <inline-formula><mml:math id="M18" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>Sv h<inline-formula><mml:math id="M19" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (reference level of exposure dose in normal times as
recommended by the ICRP). In immediate post-accidental conditions (so-called “emergency
exposure situations”), higher dose exposure levels have been allowed (the
20 mSv yr<inline-formula><mml:math id="M20" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> level was set in Japan for residency, which corresponds to
3.8 <inline-formula><mml:math id="M21" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>Sv h<inline-formula><mml:math id="M22" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> as it takes into account the fact that
people spent a maximum of 8 h d<inline-formula><mml:math id="M23" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> outdoors and 16 h d<inline-formula><mml:math id="M24" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
indoors, with indoor dose exposures being 40 % of those outdoors). A level
of 5 mSv yr<inline-formula><mml:math id="M25" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> or 2.5 <inline-formula><mml:math id="M26" display="inline"><mml:mrow class="unit"><mml:mi mathvariant="normal">µ</mml:mi></mml:mrow></mml:math></inline-formula>Sv h<inline-formula><mml:math id="M27" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> has also been defined to
enforce the individual dose control for workers (e.g. decontamination works,
working in forests) in exposed areas of Japan.</p>
      <?pagebreak page481?><p id="d1e455">As a result of the progressive radioactive decay and the associated decrease
in air dose rates with time, evacuation orders have been gradually lifted in
some areas, while they were maintained in the areas exposed to the highest
radiation dose rates (i.e. Difficult-to-Return Zone, DTRZ, or <?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g01.png"/>
in Japanese; Fig. 1). The 20 mSv yr<inline-formula><mml:math id="M28" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> threshold remained the main
guide to delineate these zones, as the so-called DTRZ corresponds to the
area where the exposure dose was expected to exceed this value even 5 years
after the accident (i.e. by 2016). To allow reopening the Special Decontamination Zone (SDZ) and DTRZ, decontamination was conducted across wide areas of Fukushima and
neighbouring prefectures in Japan, starting with the less contaminated areas
(i.e. Intensive Contamination Survey Areas, ICAs, or <?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g02.png"/> in
Japanese), followed by the SDZ (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g03.png"/> in Japanese; Evrard et al., 2019) and, finally, parts of the DTRZ (Fig. 1).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F1" specific-use="star"><?xmltex \currentcnt{1}?><?xmltex \def\figurename{Figure}?><label>Figure 1</label><caption><p id="d1e488"><bold>(a)</bold> Map of the <inline-formula><mml:math id="M29" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs deposition on soils across north-eastern
Japan following FDNPP after Kato et al. (2019a); <bold>(b–c)</bold> delineation
of the areas where decontamination works have been conducted following the FDNPP
accident in Japan including Intensive Contamination Survey Areas (40
municipalities; 7836 km<inline-formula><mml:math id="M30" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>), Special Decontamination Zone (parts of 11 municipalities; 1117 km<inline-formula><mml:math id="M31" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>) and Difficult-to-Return Zone (parts of eight municipalities; 335 km<inline-formula><mml:math id="M32" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>; source: Japanese Ministry of Environment). The corresponding shapefiles
can be freely downloaded from Evrard et al. (2023).</p></caption>
        <?xmltex \igopts{width=455.244094pt}?><graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-f01.png"/>

      </fig>

      <p id="d1e538">Decontamination was completed between 2017 and 2019 in the ICAs and in the
SDZ, with the progressive transfer of remediation waste to interim storage
facilities built in Okuma and Futaba towns (Fig. 2). After a partial
reopening in 2022, several additional portions of the DTRZ will be reopened
from 2023 onwards without obligatory decontamination except in “Special
Reconstruction and Revitalization Zones” (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g04.png"/>; Fig. 2).
Nevertheless, residential and cultivated zones of the DTRZ located outside
of these Specific Reconstruction and Revitalization Zones may be
decontaminated as well, in response to the local residents' willingness to
see their property remediated.</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F2"><?xmltex \currentcnt{2}?><?xmltex \def\figurename{Figure}?><label>Figure 2</label><caption><p id="d1e548">Detailed map of the reconstructed initial <inline-formula><mml:math id="M33" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs fallout
decay-corrected to July 2011 (Kato et al., 2019a), the municipalities of
the Difficult-to-Return Zone, the Specific Reconstruction and
Revitalization Zones and the radioactive waste management and storage
facilities (see the inset map for a close-up view on the location of these
facilities). The corresponding shapefiles can be freely downloaded from
Evrard et al. (2023).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-f02.png"/>

      </fig>

      <p id="d1e566">According to the definition given by the Japanese Ministry of Environment, a
Specific Reconstruction and Revitalization Zone is an area within the DTRZ
where environmental rehabilitation projects, such as decontamination and
house demolition, are being promoted together with infrastructure
development in order to lift the evacuation order. These zones, made
possible following Amendments made to the Fukushima Act on Special Measures
for Reconstruction and Revitalization (Act No. 25 of 31 March 2012; Cabinet Order, 2012), are set up by the mayor of the
municipality, and a plan is prepared and needs approval from the Prime
Minister. The plan is being undertaken and will be completed within 5 years of
approval, and its completion will allow the evacuation order to be lifted.</p>
      <p id="d1e569">In this unique transition context, it is timely to provide an updated
synthesis and feedback after an initial review article published in 2019
(Evrard et al., 2019) regarding the completion of this unique
remediation programme. The goal is to make the latest information available
to the international community and to identify the main challenges for
ongoing and future research at the time when the Fukushima DTRZ will be
reopened (i.e. spring 2023). Although the current article will mainly focus
on the resumption of forestry and agricultural activities in the main plume,
it will also address the impacts of decontamination on transfer of
radionuclides in different terrestrial environments. Of note, the general
transfer of radionuclides in Fukushima environments was also covered by
recent comprehensive synthesis articles (Table 1), although not with a focus
on the impact of decontamination. In contrast, the current article will not
address the fate of radioactive contamination in coastal and marine waters,
which can be found elsewhere (Table 1).</p>
      <p id="d1e573">The privileged option is rather to identify the lessons of that
unprecedented soil decontamination programme, as well as the gaps and needs
in remediation actions. After summarising the calendar for reopening, data
on people having returned and the costs of the remediation works, the
challenges for restarting soil cultivation in the remediated cropland will
be discussed. Then, focus will be laid on decontamination tests and methods
in forests, as these areas, covering ca. 75 % of the fallout-impact region,
have not been remediated at this stage (with the exception of 20 m-wide
buffer strips around houses and roads) and radionuclide cycling remains
active in these zones. Furthermore, the potential export of radionuclides
stored in soils under forests will also be addressed, as this may provide a
long-lasting source of contamination to downstream – remediated – or
non-decontaminated environments. The situation in ponds and reservoirs where
<inline-formula><mml:math id="M34" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs may be remobilised from sediment will also be examined. Finally,
the main challenges for ongoing and future research will be synthesised.</p>
</sec>
<sec id="Ch1.S2">
  <label>2</label><title>Reopening of the zones and return of previous inhabitants</title>
      <p id="d1e593">Overall, 165 000 inhabitants were evacuated from the main fallout zone in
2011, and 28 000 people remained officially considered evacuees by
November 2022 (Reconstruction Agency, 2023). The plans for
rehabilitation of six towns (Futaba, Okuma, Namie, Tomioka) and villages
(Iitate, Katsurao) in the DTRZ – submitted between September 2017 and May 2018 – were approved, and demolition/decontamination is underway or has been
completed. Evacuation orders have been lifted in spring 2022 in part of
Futaba Town (Futaba Station area), part of Okuma Town (Ono Station area),
Tomioka Town (around Yonomori Station) and Katsurao Village. Evacuation
orders were expected to be lifted in spring 2023 in similar zones in Namie
Town, Tomioka Town and Iitate Village (Fig. 2). According to an extensive
report of the Board of Audit of Japan (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g05.png"/>) published in February
2023 (Board of Audit of Japan, 2023), from the 12
municipalities of Fukushima Prefecture in which an evacuation order was
imposed in at least one neighbourhood in 2011, only 29.9 % of the 147 443 inhabitants who lived there before the accident had returned by 2020 (i.e.
44 028 inhabitants). Strong variations in the proportion of returnees were
observed, ranging from less than 5 % of the initial population in
municipalities remaining largely closed in 2020 (i.e. Futaba, Okuma,
Tomioka, Namie) up to 69.9 % in Tamura (where only a small part was
located within the DTRZ).</p>
</sec>
<sec id="Ch1.S3">
  <label>3</label><title>Progress and cost of remediation works</title>
      <p id="d1e609">Updated information related to decontamination is regularly provided in
the Japanese language on a specific website of the Japanese Ministry of
Environment (<uri>http://josen.env.go.jp/</uri>, last access: 31 August 2023), but much less
information is regularly communicated in English. For the aggregated costs,
information has been made available from the above-mentioned extensive report of
the Board of Audit of Japan published in February 2023 (Board
of Audit of Japan, 2023).</p>
      <?pagebreak page482?><p id="d1e615">The management of radioactive waste (i.e. containing at least 8000 Bq kg<inline-formula><mml:math id="M35" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> of radionuclides) depends first on the nature of the material,
i.e. whether it consists of soil/vegetation resulting from decontamination
works (referred to as category 1) or whether it consists of debris related
to the tsunami or to the demolition operations in residential settlements
(referred to as category 2; Fig. 3).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F3" specific-use="star"><?xmltex \currentcnt{3}?><?xmltex \def\figurename{Figure}?><label>Figure 3</label><caption><p id="d1e632">Procedures for the treatment of waste containing radioactive
materials from Fukushima Prefecture, after information shared by Reprun
Fukushima (Japanese Ministry of the Environment, 2023b).</p></caption>
        <?xmltex \igopts{width=341.433071pt}?><graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-f03.png"/>

      </fig>

      <p id="d1e642">For the second category of waste, a threshold of 100 000 Bq kg<inline-formula><mml:math id="M36" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> of
<inline-formula><mml:math id="M37" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs has been set to determine the disposal location of this material.</p>
      <p id="d1e666">Waste from the area where countermeasures were implemented (so-called
“specified waste”) outside of the DTRZ and with a <inline-formula><mml:math id="M38" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs content lower
than 100 000 Bq kg<inline-formula><mml:math id="M39" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> is being stored in a specific disposal site opened
in Tomioka Town on 17 November 2017 (Fig. 2). For the waste originating
from the DTRZ, it is being disposed at the Clean Centre (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g06.png"/>)
in Futaba Town as decided on 5 August 2022 (Fig. 2; Japanese Ministry of the Environment, 2023a) along with the
domestic waste produced in the eight municipalities of Futaba County
(including Hirono Town, Naraha Town, Tomioka Town, Kawauchi Town, Okuma
Town, Futaba Town, Namie Town and Katsurao Village, covering a surface
area of 866 km<inline-formula><mml:math id="M40" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>).</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T1" specific-use="star"><?xmltex \currentcnt{1}?><label>Table 1</label><caption><p id="d1e707">Selection of other review articles and reports dealing with
specific radionuclide transfer processes or remediation techniques along
with their social impacts in different environmental conditions.</p></caption><oasis:table frame="topbot"><oasis:tgroup cols="2">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="justify" colwidth="7cm"/>
     <oasis:thead>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Topic</oasis:entry>
         <oasis:entry colname="col2">References</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Continental transfer of fallout radionuclides</oasis:entry>
         <oasis:entry colname="col2">Evrard et al. (2015), Onda et al. (2020)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Environmental behaviour of fallout radionuclides</oasis:entry>
         <oasis:entry colname="col2">Nanba et al. (2022), IAEA-TECDOC-1927 (2020), Tagami et al. (2022), Nakajima et al. (2019)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Forest transfer of fallout radionuclides</oasis:entry>
         <oasis:entry colname="col2">Hashimoto et al. (2022c); Kimura (2023, 2021), Mabon (2019)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Impact of radionuclides on freshwater environments</oasis:entry>
         <oasis:entry colname="col2">Nagao (2021), Asanuma-Brice et al. (2023)</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1">Impacts of radionuclides on agriculture</oasis:entry>
         <oasis:entry colname="col2">Nakanishi and Tanoi (2016), Kuroda et al. (2021), Vandenhove and Turcanu (2016)</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Oceanic transfer of fallout radionuclides</oasis:entry>
         <oasis:entry colname="col2">Buesseler et al. (2017), Xixi et al. (2022), Mabon and Kawabe (2022)</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup></oasis:table><?xmltex \gdef\@currentlabel{1}?></table-wrap>

      <p id="d1e789">Regarding the waste resulting from decontamination (soil and vegetation;
category 1), as of 7 March 2023 (Japanese Ministry of the
Environment, 2023a), the progress of these operations has exceeded 90 %,
with the latest work being completed in the Special Reconstruction and
Revitalization Zones of the DTRZ.</p>
      <p id="d1e792">Out of a total of 1372 temporary storage sites scattered across the
landscapes in Fukushima Prefecture, by February 2023, 31 sites were
still storing soil to be removed, 1341 had seen their waste being
completely removed, and 1070 temporary storage sites had been restored to
their original state. Waste amounting to 13.43 million m<inline-formula><mml:math id="M41" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> was transported to interim storage facilities. The soil removed from these sites
was sorted and processed, and as of late February 2023, approximately 11.54 million m<inline-formula><mml:math id="M42" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">3</mml:mn></mml:msup></mml:math></inline-formula> of this waste was stored at the interim storage facilities.
Furthermore, 17 382 steel rectangular containers filled with ash dust mainly
resulting from biomass combustion were stored at the same facilities by
February 2023. At the end of January 2023, approximately 1.42 million t
of waste had been treated at each at the temporary incineration facilities
operated by national authorities. Wood crushers are being used to limit the
volume of waste from forests (with corresponding volume reduction rates
between 45 % and 63 %), and combustible waste (i.e. fallen leaves and branches)
is being incinerated at these temporary facilities with a very high volume
reduction (96 %–99 %) and a very low transfer of <inline-formula><mml:math id="M43" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs to exhaust air
(<inline-formula><mml:math id="M44" display="inline"><mml:mo lspace="0mm">≤</mml:mo></mml:math></inline-formula> 0.3 Bq m<inline-formula><mml:math id="M45" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">3</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>; Hashimoto et al., 2022a). Special attention is
nevertheless being required for the subsequent management of combustion ash
with high <inline-formula><mml:math id="M46" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations (<inline-formula><mml:math id="M47" display="inline"><mml:mi mathvariant="italic">&gt;</mml:mi></mml:math></inline-formula> 2 000 000 Bq kg<inline-formula><mml:math id="M48" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>).</p>
      <?pagebreak page483?><p id="d1e871">In accordance with the Act on Special Measures Concerning the Handling of
Contamination by Radioactive Substances, specified waste containing more
than 100 000 Bq kg<inline-formula><mml:math id="M49" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> of <inline-formula><mml:math id="M50" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs is also being stored at these
interim storage facilities in Okuma and Futaba towns, which became operational
in October 2017. These facilities covered a total area of 1285 ha acquired
from 1853 land owners by late February in 2023 (orange surface areas in
Fig. 2). According to the Japanese law, this material is supposed to be
transported to final disposition sites located outside of Fukushima
Prefecture at locations that remain to be selected by 2047 (i.e. 30 years
after the interim storage facilities became operational).</p>
      <p id="d1e895">The costs of the recovery and reconstruction operations conducted by the
Japanese authorities following the Great East Japan Earthquake and the
associated nuclear accident at FDNPP during the period between
2011 and 2020 were recently synthesised by the Board of Audit of Japan in
February 2023 (Board of Audit of Japan, 2023). A conversion
rate of EUR 1 <inline-formula><mml:math id="M51" display="inline"><mml:mo>=</mml:mo></mml:math></inline-formula> JPY 140   (as of 1 January 2023) was used in the
current text. They estimated that the total of these costs reached JPY 38 171.1 billion (<inline-formula><mml:math id="M52" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> EUR 273 billion), with a provisioned and
remaining budget of JPY 6144 billion (<inline-formula><mml:math id="M53" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> EUR 44 billion).
Among these costs, 20 % of the budget (JPY 7745.6 billion; <inline-formula><mml:math id="M54" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> EUR 55 billion) was devoted to reconstruction/public works and 16 % of
the budget (JPY 6122.3 billion; <inline-formula><mml:math id="M55" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> EUR 44 billion) was spent
on the “nuclear recovery policy” including decontamination. Most of the
provisioned and unused budget by 2020 is expected to be spent on
reconstruction/publics works (34 % of residual budget; JPY 2094 billion;
<inline-formula><mml:math id="M56" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> EUR 14 billion) and nuclear recovery (22 %; JPY 1343.9 billion; <inline-formula><mml:math id="M57" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> EUR 9.6 billion). For the period between
2011 and 2020, as the annual budget of the State of Japan varied around
<inline-formula><mml:math id="M58" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> JPY 90 000–100 000 billion
(<inline-formula><mml:math id="M59" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> EUR 700–800 billion), this demonstrates that the budget
spent on the reconstruction following the Great East Japan Earthquake and
the associated nuclear accident at FDNPP was far from negligible.</p>
</sec>
<sec id="Ch1.S4">
  <label>4</label><title>Recultivation of cropland</title>
      <p id="d1e970">In the least contaminated cropland fields (with typical <inline-formula><mml:math id="M60" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
activities <inline-formula><mml:math id="M61" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 5000 Bq kg<inline-formula><mml:math id="M62" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>), tillage and topsoil/subsoil
interchange provided a common countermeasure (Evrard et al.,
2019). A study conducted at an experimental site of the ICA (Ibaraki
Prefecture) between 2011 and 2017 confirmed that <inline-formula><mml:math id="M63" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in
both soils and crops (i.e. soybean) decreased exponentially with time
elapsed since the accident as a result of tillage operations (Li et al.,
2019). In contrast, in paddy fields and other cropland with <inline-formula><mml:math id="M64" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
levels exceeding 5000 Bq kg<inline-formula><mml:math id="M65" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (covering a surface area of
<inline-formula><mml:math id="M66" display="inline"><mml:mo>∼</mml:mo></mml:math></inline-formula> 827 km<inline-formula><mml:math id="M67" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> in Fukushima
Prefecture; Nakanishi, 2018), a major countermeasure for soil
decontamination has generally consisted in the removal of the 5 cm upper
layer concentrating radiocesium. In the SDZ and DTRZ, the addition of crushed granite and/or saprolite extracted
locally and its mixing with the residual initial soil profile compensated for soil removal
(Evrard et al., 2019). In the official reports and guideline
books, this practice is justified by the need to supply “fresh”, “clean”
or “new” soil “in order to ensure the conditions that enable resumption
of agricultural production are restored”(Japanese
Ministry of Environment, 2013). However, this decontamination process may
have led to a decrease in fertility of these soils and enhanced erosion,
with strong heterogeneities within the fields (Inoue et al., 2020).
Technical developments are currently under progress to contribute to the
rapid assessment of soil fertility in this context based on hyperspectral
reflectance measurements (400–2500 nm) of soil samples, and the subsequent
calculation of spectral index algorithms (Inoue et al., 2020).</p>
      <p id="d1e1048">Another commonly applied countermeasure is the application of potassium (K)
fertilisers in order to promote K–Cs (as<?pagebreak page484?> an analogue) competition at the
soil solution–root interface and reduce the root uptake of radiocesium by
crops (Zhu and Smolders, 2000). The positive effect of potassium
fertiliser on radiocesium transfer to vegetation has been widely studied in
post-Chernobyl studies; this countermeasure is most effective in soils with
naturally low levels of exchangeable potassium. As a remedial action in
contaminated soils of Fukushima Prefecture, increasing exchangeable
potassium up to 25 mg K<inline-formula><mml:math id="M68" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O 100 g<inline-formula><mml:math id="M69" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in soil was recommended for
agricultural soils where the concentration of exchangeable potassium was
below that level (Japanese Ministry of Agriculture,
2013). Furthermore, recent research based on field experiments demonstrated
that a complementary soil property (i.e. non-exchangeable K) and a level of
<inline-formula><mml:math id="M70" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 50 mg K<inline-formula><mml:math id="M71" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O 100 g<inline-formula><mml:math id="M72" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> could be used as another threshold for
use along with that of exchangeable K (<inline-formula><mml:math id="M73" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 25 mg K<inline-formula><mml:math id="M74" display="inline"><mml:msub><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msub></mml:math></inline-formula>O 100 g<inline-formula><mml:math id="M75" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) to identify soils that would need additional K fertilisation
(Kurokawa et al., 2020). Another field of research is devoted to the
optimisation of agricultural practices for the K budget. For example,
Nishikiori et al. (2020) investigated the plant-available K budget at the
field scale by comparing two fields with different soil textures and
drainage conditions. The major inputs of K to the fields were shown to be
fertilisation, straw return and irrigation, while the major outputs were
plant harvesting, surface runoff and water percolation. Nevertheless, most K
harvested with the plants (85 %) was brought back to the soil by straw
return. In contrast, water percolation and surface runoff were the dominant
output pathways, with most of K being discharged from the fields before
mid-summer drainage, contributing significantly to the general negative K
balance (comprising <inline-formula><mml:math id="M76" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>20 to <inline-formula><mml:math id="M77" display="inline"><mml:mo>-</mml:mo></mml:math></inline-formula>289 kg ha<inline-formula><mml:math id="M78" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). Careful irrigation
adapted to the soil conditions is thus recommended to reach a more
appropriate K budget in soils in order to limit the radiocesium transfer to
plants.</p>
      <p id="d1e1155">The potential transfer of radiocesium via irrigation water in paddy fields
also remains a matter of concern. The monitoring of total and dissolved
radiocesium in irrigation water, rice and soil from two decontaminated paddy
fields showed that 85 % of radiocesium in irrigation water was not
exported and remained in the field (Shin et al., 2019). However, the
quantity of additional radiocesium supplied by irrigation water was
negligible (<inline-formula><mml:math id="M79" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 0.08 % of the initial inventory) compared to
the initial supply by radioactive fallout in 2011. This resulted in very low
soil to brown rice transfer factors of radiocesium (0.0015–0.0068).</p>
      <p id="d1e1165">In parallel to these studies investigating the transfer of radionuclides in
cultivated land, strict controls were implemented by Japanese authorities to
monitor radiocesium concentrations in food products. Accordingly, between
2012 and 2021, more than 2.5 million samples of food products were analysed
for radiocesium (Nakamura et al., 2022). The
Japanese radiocesium permitted levels (i.e. 100 Bq kg<inline-formula><mml:math id="M80" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for general
foodstuff and 10 Bq kg<inline-formula><mml:math id="M81" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for drinking water) were not exceeded in more
than 99 % of samples. Despite these low levels of contamination detected in foodstuff,
Japanese food shipping restrictions remained imposed by many countries
(including the European Union following Regulation 2016/6, China and South
Korea) as of 2023, despite the US Food and Drug Administration (FDA)
deactivating its import alert in September 2021 (US FDA, 2023).</p>
</sec>
<sec id="Ch1.S5">
  <label>5</label><title>Radionuclide cycling in forests and contamination of forest products</title>
      <?pagebreak page485?><p id="d1e1201">The situation in forests should receive particular attention, as they
cover 71 % of the surface of Fukushima Prefecture (ca. 970 000 ha; Hashimoto et al., 2022c). Evergreen coniferous trees (Japanese cedar –
<italic>Cryptomeria japonica</italic>, Japanese cypress – <italic>Chamaecyparis obtusa</italic>, red pine – <italic>Pinus densiflora</italic>) used for construction timber account
for about 40 % and deciduous trees (konara oak – <italic>Quercus serrata</italic>) – mainly for
paper-making materials and mushroom cultivation – for about 60 %
(Hashimoto et al., 2022d). Before the FDNPP accident, the Abukuma Highlands were
actively used for cultivating trees (mainly konara oak) for producing
mushroom logs.</p>
      <p id="d1e1216">The FDNPP accident atmospheric fallout was at the origin of the
contamination of 2600 km<inline-formula><mml:math id="M82" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> of forests, with radiocesium levels
exceeding 100 kBq m<inline-formula><mml:math id="M83" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>, which should be compared to the
360 km<inline-formula><mml:math id="M84" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> surface area of cropland affected by those levels
(Onda et al., 2020). Overall, 60 %–90 % of radiocesium that fell on
cedar and cypress forests was first intercepted by the canopy (leaves and
branches) and partially absorbed by the foliage. In contrast, the leaves of
deciduous trees had not burst yet, and the level of fallout trapping was
therefore lower in broadleaf forests (Hashimoto et al., 2022b; Kato et
al., 2019b). Then, radiocesium was rapidly transferred by water (throughfall
and stemflow) and defoliation (litterfall) towards the forest floor and the
underlying mineral soil, which represented the most important pools of
radiocesium a few years after the accident. Vertical redistribution of
radiocesium between the forest floor and mineral layers was established within
1–2 years of fallout and changed slowly thereafter. The rapid
accumulation in topsoil layers is likely related to the relatively wet
climate, which promoted the early vertical migration of radiocesium in
numerous Japanese forests. In the mineral soil layer, radiocesium is firmly
retained on mineral soil particles and its content peaks at shallow depths
(typically <inline-formula><mml:math id="M85" display="inline"><mml:mi mathvariant="italic">&lt;</mml:mi></mml:math></inline-formula> 5 cm; Hashimoto et al., 2022b). However, despite
the current low migration with depth, bioturbation by organisms may also
contribute to further soil and associated radiocesium transfer across the
soil profile.</p>
      <p id="d1e1256">In contaminated forests, both the forest floor and the topsoil layers now
represent significant reservoirs of radiocesium available for root uptake by
trees and understorey species. That phenomenon is the predominant cause of
the long-term radiocesium recycling associated with the biomass turnover and
that of a possible long-lasting contamination of forest products
(Goor and Thiry, 2004). Variability in stemwood
contamination (i.e. the trunk excluding the bark) is expected to depend on
various factors: time after fallout, tree species and age, position in the
stand, radiocesium and K contents in the soil, etc. (Ohashi et al.,
2020). Initial vertical and radial movement of radiocesium within the
stemwood and its redistribution between sapwood and heartwood have been
variable, depending mainly on tree species (Ota and Koarashi, 2022).
Radiocesium content and distribution in stemwood of both coniferous and
deciduous trees is now approaching the equilibrium state, although higher
<inline-formula><mml:math id="M86" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in heartwood of cedars compared to oaks remain
under investigation (Hashimoto et al., 2022b). An aggregated transfer
factor for different major tree species has been proposed to calculate the
tree organs contamination in radiocesium taking into account the total
surface contamination levels estimated by airborne surveys
(Hashimoto et al., 2020c). However, the proportion of
radiocesium remaining in the forest floor of different forests remains quite
variable (Imamura et al., 2020), which may induce uncertainty in further
recycling by trees as radiocesium found in the organic layer (devoid of clay
minerals) is usually much more bioavailable for root uptake (Thiry et
al., 2000). Field monitoring of radiocesium bioavailability in soils was
conducted at two neighboured forest sites (one with Japanese cedar, the
other with konara oak) in Kawauchi Village between 2011 and 2017 (Manaka et
al., 2019). An exponential decrease in the proportion of exchangeable
<inline-formula><mml:math id="M87" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs was observed in organic and mineral soil layer samples at both
sites. The proportion significantly decreased within 2–4 years of the
accident, becoming almost constant thereafter (2 %–4 %). These<?pagebreak page486?> results
support the interpretation that contaminated forests have entered a
steady-state phase of <inline-formula><mml:math id="M88" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs cycling. Several articles on tree
contamination with time have been published in recent years and they all
confirm similar findings, which increases our confidence in these results
(Gonze et al., 2021; Yoschenko et al., 2022).</p>
      <p id="d1e1286">The fate of radiocesium cycling in forests can also be anticipated with
numerical modelling. Recent simulations have shown that initial foliar
absorption by coniferous trees and subsequent internal transfer promote
radiocesium persistence in trees and thus have a strong possible impact
on the early phasing of tree contamination (Thiry et al., 2018, 2020). The simulated contributions of foliage and root uptake to
tree contamination were equivalent 10–15 years after the atmospheric
deposits, but the further root uptake was too low to compensate for the activity
decline in the tree with time. In a model inter-comparison for Japanese
forests (Hashimoto et al., 2020a), convergent simulations confirmed that
an equilibrium state in tree wood contamination is reached ca. 10 years
after the initial fallout, even in konara oaks, and that they then decline
slowly. The highest uncertainty in the simulations of wood contamination
remains for newly planted trees, where root uptake is the only pathway.
These results indicated that the parameterisation of long-term net root
uptake remains uncertain without additional field monitoring.</p>
      <p id="d1e1290">Although there is no restriction on the use of wood as a building material,
wood contamination in particular represents a problem for log production for
mushroom cultivation and fuel chip production, not only in Fukushima
but also in neighbouring prefectures (due to the lower
<inline-formula><mml:math id="M89" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs limits – 40 or 50 Bq kg<inline-formula><mml:math id="M90" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> maximum – allowed for these uses of
wood; see Table 2). Debarking of trunks can lower <inline-formula><mml:math id="M91" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations
to allow wood to be used for biofuel production, although care will have
to be taken to manage the resulting ashes (Hashimoto et al., 2022a). Technology for methane fermentation of contaminated wood biomass has also
been tested (Hashimoto et al., 2022b), with the methane gas produced devoid
of radiocesium, which was recovered instead in the fermentation digestate.
However, decontaminating digestate before use as a common fertiliser
remains problematic (Kobayashi et al., 2020).
New challenges may involve the management of abandoned contaminated fields
and certain waste substrates using new forests or short rotation coppice
dedicated to bio-fuel production. This implies the in situ radiological control of
radiocesium cycling on long timescales through appropriate and sustainable
methods of biomass cultivation adapted to the Japanese ecological conditions
and its conversion into energy as it was tested in post-Chernobyl studies
(Vandenhove et al., 2001; Thiry et al., 2001) and, more recently, in
post-Fukushima experiments (Kobayashi et al., 2013). Tree log soaking
and/or further wood chip/sawdust washing in presence of a suitable
radiocesium absorbent (e.g. Neda, 2013), represent other potential
countermeasures, which still need to be tested or improved for the Fukushima
conditions. For forests contaminated around Chernobyl, the study of  Shaw et al. (2001) revealed that a cost-effective management strategy would also require
novel alternative uses of forest products, which could provide added value
to the standing crop in return for a small increase in public and worker
doses. In that context,  Dubourg (1996) recommended a radiological
clean-up approach involving both the incineration of the most contaminated
parts of the tree and the branches, and the transformation into paper pulp
of the less contaminated part of the trunk. Another idea that emerged after
the Chernobyl accident but that was never tested (Yves Thiry, personal communication, 2023) and that remains debated would imply a shift in the local use of wood
products through e.g. the production of wood shingles after a special
treatment of standing coniferous trees through debarking. As practised in
Scandinavia from the early medieval period, debarking provokes the
decline of the tree together with the resination of the stemwood. After
several years of tree decline, the natural impregnation of the timber is
supposed to be associated with a loss of potassium in stemwood and by
analogy with a removal of radiocesium. Shingling (<italic>itabuki</italic>, <?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g07.png"/>) using cedar wood was
widely used in forest areas of Japan and even in urban areas until the end
of the Edo period (1603–1867; Japanese Architecture and Art
Net Users Systems, 2001). Hopefully, by promoting a natural decontamination
of wood, such a practice, once adapted, could also provide a source of
added value and revitalisation for the local wood industry in contaminated
forest areas.</p>

<?xmltex \floatpos{t}?><table-wrap id="Ch1.T2"><?xmltex \currentcnt{2}?><label>Table 2</label><caption><p id="d1e1334">Current radiocesium threshold values for forest products in Japan,
after Hashimoto et al. (2022b).</p></caption><oasis:table frame="topbot"><?xmltex \begin{scaleboxenv}{.88}[.88]?><oasis:tgroup cols="2">
     <oasis:colspec colnum="1" colname="col1" align="left"/>
     <oasis:colspec colnum="2" colname="col2" align="right"/>
     <oasis:thead>
       <oasis:row>
         <oasis:entry colname="col1">Forest product</oasis:entry>
         <oasis:entry colname="col2">Maximum radiocesium</oasis:entry>
       </oasis:row>
       <oasis:row rowsep="1">
         <oasis:entry colname="col1"/>
         <oasis:entry colname="col2">concentration (Bq kg<inline-formula><mml:math id="M92" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>)</oasis:entry>
       </oasis:row>
     </oasis:thead>
     <oasis:tbody>
       <oasis:row>
         <oasis:entry colname="col1">Tree logs for shiitake cultivation</oasis:entry>
         <oasis:entry colname="col2">50</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Sawdust medium for mushroom cultivation</oasis:entry>
         <oasis:entry colname="col2">200</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Firewood (for cooking)</oasis:entry>
         <oasis:entry colname="col2">40</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Charcoal (for cooking)</oasis:entry>
         <oasis:entry colname="col2">280</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Wood pellets</oasis:entry>
         <oasis:entry colname="col2">40</oasis:entry>
       </oasis:row>
       <oasis:row>
         <oasis:entry colname="col1">Bark compost for livestock bedding</oasis:entry>
         <oasis:entry colname="col2">400</oasis:entry>
       </oasis:row>
     </oasis:tbody>
   </oasis:tgroup><?xmltex \end{scaleboxenv}?></oasis:table><?xmltex \gdef\@currentlabel{2}?></table-wrap>

      <p id="d1e1436">Mushroom and wild plant contamination is still particularly problematic in a
country where the hunt for mushrooms and wild/mountain
vegetables is so popular both as a popular leisure activity or part of
cultural traditions (offerings for Obon (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g10.png"/>) Festival in August or New Year's
Day). Satoyama (<?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g08.png"/>) traditions are widespread in mountainous rural zones
located in the vicinity of forests in Japan where people live in harmony
with nature and collect edible food from forests (including plants –
referred to as sansai or <?xmltex \igopts{height=8.535827pt}?><inline-graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-g09.png"/> – and mushrooms). Because of the high
contamination found in forests and its static character, the absence of
decontamination and the ability of these organisms to absorb radiocesium
efficiently, they represent the vast majority of food products exceeding the
standard limit of 100 Bq <?pagebreak page487?>kg<inline-formula><mml:math id="M93" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> (Hori et al., 2018), with the
dominance of wild plants in spring and that of mushrooms in autumn
(Hashimoto et al., 2022a). As of November 2020, shipping restrictions on
mushrooms had been imposed by 117 municipalities in 11 prefectures (Fig. 4).</p>
      <p id="d1e1466">It is impossible to provide a comprehensive list of species to avoid
collecting, as there are 4000–5000 species of wild mushrooms in Japan.
Nevertheless, a study showed that although 76 % of the mushrooms collected
between 2016 and 2019 in Kawauchi Village, located near the DTRZ, exceeded the
maximum allowed threshold of 100 Bq kg<inline-formula><mml:math id="M94" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in <inline-formula><mml:math id="M95" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs, the committed
effective dose due to consuming mushrooms was lower than 1 mSv yr<inline-formula><mml:math id="M96" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>
(Cui et al., 2020).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F4"><?xmltex \currentcnt{4}?><?xmltex \def\figurename{Figure}?><label>Figure 4</label><caption><p id="d1e1504">Map of the Japanese municipalities with mushroom shipping
restrictions as of November 2022 after  Hashimoto et al. (2022a). The
corresponding shapefiles can be freely downloaded from Evrard et
al. (2023).</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-f04.png"/>

      </fig>

      <p id="d1e1514"><inline-formula><mml:math id="M97" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in mushrooms were found to be related to the soil
contamination, and normalised concentrations allow comparisons between
regions/species. In general, as observed in forests contaminated around Chernobyl,
mycorrhizal fungi living in symbiosis with trees have higher <inline-formula><mml:math id="M98" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations than saprotrophic fungi, obtaining their nutrients from
decomposing dead wood and leaves (Komatsu et al., 2019). However, this
general result was counterbalanced by the fact that some species showed different behaviour, which justifies the general prohibition of all
mushrooms in a wide area across north-eastern Japan as a matter of
precaution. In a similar way as for wild mushrooms, <inline-formula><mml:math id="M99" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations were found to be strongly variable in wild plants, with some
plants showing noticeably higher contamination levels, e.g. koshiabura
(<italic>Eleutherococcus sciadophylloides</italic>), and some cooking techniques were found to be effective to decrease
<inline-formula><mml:math id="M100" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs levels in wild plants, e.g.  Hashimoto et al. (2022a). There
has also been a large impact in recreational activities, with a large
decrease in the number of climbers and fishers visiting Fukushima
Prefecture, along with a similar decrease in the number of urban visitors.</p>
      <p id="d1e1555">In addition to wild mushroom picking, mushroom cultivation is very popular
in Japan and it represented 80 % of non-wood forestry production in
2017 (i.e. non-wood forestry production excluding timber, which
accounted for 43 % of total forestry production in Japan). Two
techniques are used, i.e. bed-log cultivation (mainly used for
shiitake production) and sawdust medium cultivation, with the second technique
having become increasingly dominant in recent decades in Japan (as it is less
labour consuming and given the increasing preference of the Japanese
population for mushrooms other than shiitake). Of note, wood-log standards are more
stringent than those associated with sawdust, and the concentration of
sawdust can then be adjusted to meet the standards. The increase in sawdust
cultivation was further accentuated after the FDNPP accident, with the
restriction of the production and shipment of shiitake mushrooms across a
wide area in Japan. The problem is that wood (mainly of konara oak –
<italic>Quercus serrata</italic>) from Fukushima Prefecture (e.g. Abukuma Mountains) was not only used
for the local production of shiitake but also to provide mushroom logs used for
the production carried out in other Japanese prefectures. This production
had to be stopped because of the very high levels of <inline-formula><mml:math id="M101" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs (up to more
than 10 times the index value) recorded in the production region
(Hashimoto et al., 2022a). Interestingly, as observed for cultivated
soils, a strong negative correlation was observed between radiocesium
concentrations in the most recent branches of konara oak and exchangeable K
in the soil surface (0–5 cm depth) layer (Kanasashi et al., 2020). Since
mushroom log production requires a 20-year cycle, long-term monitoring may
open the way to better use of konara oaks grown on soils with high
concentrations of exchangeable K to produce less-contaminated or even uncontaminated
wood.</p>
</sec>
<sec id="Ch1.S6">
  <label>6</label><title>Decontamination of forests</title>
      <p id="d1e1578">Forest decontamination methods can be subdivided into two groups: (i) the
measures actually implemented in Fukushima impact zones and (ii) those
evaluated for research or practical issues. Regarding (i), only the area located
within 20 m of the forest edges (bordering residential areas, roads and
other living areas) were treated. In this buffer zone, the<?pagebreak page488?> vegetation and
contaminated organic layer (litter and humus) is gathered and transported
out of forests. Among the potential methods investigated although not
implemented widely (ii), the removal of the forest floor litter layer had
soon been considered as a potential method for reduction in tree
contamination in experimental studies. Removal of the forest floor was likely to
be more useful when operated after the peak of the transfer of radiocesium from
the aboveground parts of trees to the organic layer (Thiry et al.,
2018). This peak typically occurs around 3–5 years after the initial
deposition, although the time period varies with tree species and soil
organic layer characteristics (IAEA-TECDOC-1927, 2020). Koarashi et al. (2020) tested the impact of litter removal conducted in a broadleaf forest
in July 2014 (i.e. more than 3 years after the accident). They observed no
effect on tree contamination and a decrease of litter <inline-formula><mml:math id="M102" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
contamination in the first year following remediation and suggested that
this method should be applied even more rapidly (within 1–2 years) after
the accident, before the significant transfer of <inline-formula><mml:math id="M103" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from litter to
the underlying mineral soil. For coniferous stands, Thiry et al. (2018)
indicated a low response of tree contamination to litter removal even in the
long term because the initial <inline-formula><mml:math id="M104" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs foliar absorption is more
influential than the root pathway for a long time.</p>
      <p id="d1e1608">In addition, clear-cutting (i.e. cutting all trees) and thinning (i.e.
partial cutting) can be implemented; however, their additional contribution
to decrease air dose rates could not be demonstrated. Potassium
fertilisation can therefore be used to limit the absorption of radiocesium
by plants, as demonstrated for konara oaks (Kobayashi et al., 2019).</p>
      <p id="d1e1611">In parallel to these decontamination issues, it should be stressed that the
absence of forest management in human-made forests can lead to other problems,
such as the spread of insects and diseases. Forest maintenance includes
planting, clearing, thinning and maintenance of forest roads, which are
crucial to avoid a degradation of different forest functions (e.g. carbon
sequestration, wood production, landslide control). Moreover, thinning and
other particular silviculture treatments remain important for reducing fuel
load and fire hazard, or just for implementing strategic fuel breaks – i.e.
through converting one strip of land from one vegetation type to another for
firefighting purposes, as experimented in Chernobyl forests (Ager
et al., 2019). Still, the forest area which has been maintained in Fukushima Prefecture has decreased by ca. 50 % from 2011 onwards as a
result of the access restrictions due to high dose rates (Hashimoto et
al., 2022a). Restrictions have also been imposed on the shipping of wildlife
meat (i.e. wild boar, Asian black bear, sika deer, spot-billed duck, green
pheasant, copper pheasant) in Fukushima and/or nearby
prefectures because of their excessive <inline-formula><mml:math id="M105" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs muscle contamination.
These shipping restrictions along with a decrease of hunter numbers and
of capture pressure (i.e. number of captures per hunter) observed all
across Japan led to wildlife population expansion. Wild boar proliferation,
in particular, leads to extensive damage to houses and crops in the main
<inline-formula><mml:math id="M106" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs-fallout-impacted area (Hashimoto et al., 2022a). A recent
study analysed <inline-formula><mml:math id="M107" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in wild boar muscle samples
(<inline-formula><mml:math id="M108" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">221</mml:mn></mml:mrow></mml:math></inline-formula>) collected from the DTRZ and surrounding areas between 2016 and
2020. This research outlined higher activity concentrations observed in the
DTRZ compared to the surrounding areas, and an overall decrease of
<inline-formula><mml:math id="M109" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs values with time (Saito et al., 2022). Seasonal variations in
<inline-formula><mml:math id="M110" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs muscle concentrations were also observed, and these may be
related to changing food habits and the fractions of available <inline-formula><mml:math id="M111" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in
the material ingested by wild boars (Saito et al., 2020). Nevertheless,
these seasonal variations were shown to be less pronounced than in wild
boar contaminated in Germany following the Chernobyl accident, and this
observation may be due to their more diverse food sources in
Japan (Berendes and Steinhauser, 2022). Overall, as the <inline-formula><mml:math id="M112" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
contamination in wildlife muscles decreases with the distance from FDNPP,
the strategy may be two fold. First, in areas farther from FDNPP, where
muscle contamination is likely to remain below the standard limit of 100 Bq kg<inline-formula><mml:math id="M113" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> for meat consumption, shipping of the meat may be authorised after
inspection of all slaughtered individuals conducted at special facilities
specifically designed to this end in Tochigi and Ibaraki prefectures.
Second, in the areas close to FDNPP, where this threshold is expected to be
exceeded for a long time and where wildlife population is expanding, active
extermination (by hunting or capture) and subsequent incineration of
the bodies should be considered (Hashimoto et al., 2022a).</p>
</sec>
<sec id="Ch1.S7">
  <label>7</label><title>Export of radionuclides from forest to riverine ecosystems</title>
      <p id="d1e1710">Forests that remain contaminated with <inline-formula><mml:math id="M114" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs may supply contamination to
lower landscape areas. A study showed that dissolved <inline-formula><mml:math id="M115" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations measured in a stream draining a forested headwater catchment
was mainly derived from soil water with high dissolved <inline-formula><mml:math id="M116" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations originating from litter leachate. When storms occur, with the
expansion of soil saturated zones, an increase in dissolved <inline-formula><mml:math id="M117" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations coinciding with the release of water stored in shallow soil
layers is observed (Iwagami et al., 2019). This additional supply
of dissolved <inline-formula><mml:math id="M118" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from forest litter has been confirmed by leaching
tests conducted on broadleaf litter in an area affected by saturation
overland flow during storm events (Sakakibara et al., 2021).</p>
      <p id="d1e1758">Different pathways of radiocesium transfer from forests to river systems can
be found, i.e. via litter fall into rivers, lateral inflow from the forest
litter layer, and lateral transfer from the underlying forest soil. In a
modelling exercise,  Kurikami et al. (2019) showed that the decreasing
trend of <inline-formula><mml:math id="M119" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in river water and freshwater fish was due to a
combination of the decreasing contamination trend in the forest
leaves/needles and litter compartments, and the increasing contamination
trend in soil.</p>
      <?pagebreak page489?><p id="d1e1770"><?xmltex \hack{\newpage}?>When clear-cutting is conducted, suspended sediment exports were found to
increase two fold, with a much more limited increase in <inline-formula><mml:math id="M120" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs export
due to the very high sediment contribution of areas with low <inline-formula><mml:math id="M121" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations, e.g. channel bank erosion (Nishikiori
et al., 2019).</p>
      <p id="d1e1792">Another approach relied on the use of a mass balance model to map the
spatial distribution of <inline-formula><mml:math id="M122" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs inventories and quantify <inline-formula><mml:math id="M123" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
transport via sediment and litter in 2016–2017 along a deciduous forested
hillslope of Date, in Fukushima Prefecture (Oda et al., 2022).
They showed that <inline-formula><mml:math id="M124" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs inventories were significantly higher in
downslope riparian areas (455 kBq m<inline-formula><mml:math id="M125" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) than in the upslope ridge area
(179 kBq m<inline-formula><mml:math id="M126" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">2</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). Annual <inline-formula><mml:math id="M127" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs transport with litter and sediment
corresponded to less than 0.5 % of the <inline-formula><mml:math id="M128" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs hillslope inventory, and
transport of litter with high <inline-formula><mml:math id="M129" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activity concentrations was found
to provide the main pathway of <inline-formula><mml:math id="M130" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs transfer at that scale.</p>
      <p id="d1e1884">Nevertheless, this transfer of <inline-formula><mml:math id="M131" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in forest environments, although
significant in terms of export of contaminated material, was not shown to
have an impact on radiation dose rates in forests, as shown by the
monitoring of radiation levels along a hiking trail across forests in
Tomioka Town in 2019, which remained stable despite the occurrence of the Hagibis super typhoon in October 2019 (Taira et al., 2020).</p>
</sec>
<sec id="Ch1.S8">
  <label>8</label><title>Impacts of decontamination in radionuclide activities in riverine systems</title>
      <p id="d1e1904">Multiple recent publications have confirmed that <inline-formula><mml:math id="M132" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in
river water and in sediment transported in rivers draining the main
radioactive pollution plume strongly decreased between 2011 and 2020, and
some of these datasets are available in open access (Taniguchi et al.,
2020; Evrard et al., 2021). A database compiling <inline-formula><mml:math id="M133" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activities
measured in sediment (<inline-formula><mml:math id="M134" display="inline"><mml:mrow><mml:mi>n</mml:mi><mml:mo>=</mml:mo><mml:mn mathvariant="normal">782</mml:mn></mml:mrow></mml:math></inline-formula>) collected from 27 to 71 locations during 16
fieldwork campaigns conducted between November 2011 and November 2020 across
catchments (6450 km<inline-formula><mml:math id="M135" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> ) draining the main radioactive
pollution plume of Fukushima Prefecture demonstrated that the
radiocesium levels in sediment transiting these rivers decreased by more
than 90 % between 2011 and 2020 (Evrard et al., 2021).</p>
      <p id="d1e1946">Interestingly, very similar results were obtained based on continuous and
more detailed monitoring in local upper catchments of the region. Fluvial
discharge of <inline-formula><mml:math id="M136" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs was monitored between 2011 and 2021 from two small
rivers: Hiso River, draining mainly farmland (4 km<inline-formula><mml:math id="M137" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>), and Wariki River, draining mainly forests (7 km<inline-formula><mml:math id="M138" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula>), in Iitate Village (Ueda et al., 2021). Both
particulate and dissolved <inline-formula><mml:math id="M139" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations – particulate fluxes
representing 90 % of the total <inline-formula><mml:math id="M140" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs export – were shown to have
decreased very strongly, by more than 90 % over a 10-year period (with
higher decreases observed in the catchment dominated by farmland than in
that dominated by forests).</p>
      <p id="d1e1994"><?xmltex \hack{\newpage}?>In the main river of the region (i.e. Abukuma River, draining ca. 5300 km<inline-formula><mml:math id="M141" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">2</mml:mn></mml:msup></mml:math></inline-formula> of land, characterised by heterogeneous initial <inline-formula><mml:math id="M142" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
deposition levels), Taniguchi et al. (2019) found that the high
<inline-formula><mml:math id="M143" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations observed in suspended sediment just after the
accident in 2011 showed a steep exponential decline that lasted for about
1 year and that was dominated by the supply of <inline-formula><mml:math id="M144" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from paddy
fields, other farmland and urban areas. This initial phase was followed by a
more gradual secondary decline, with a higher contribution of <inline-formula><mml:math id="M145" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
from forests. Overall, the particulate form of <inline-formula><mml:math id="M146" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs represented
96.5 % of the exports investigated in this study between June 2011 and
August 2015.</p>
      <p id="d1e2053">Decontamination works conducted in farmland and residential areas took place
from 2013 to 2018 in the Special Decontamination Zone, including in those
areas located near Niida River, flowing across Iitate Village and
Minamisoma Town. A study combining river monitoring with governmental
decontamination data and high-resolution satellite images provided a
comprehensive impact assessment of these remediation works. Feng et al. (2022) showed the occurrence of two phases, with a first stage of increase
in erosion (<inline-formula><mml:math id="M147" display="inline"><mml:mo lspace="0mm">+</mml:mo></mml:math></inline-formula>237 %) during decontamination (2013–2016) – when soils
were left bare to remove the topsoil surface layer concentrating <inline-formula><mml:math id="M148" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
– followed by a decrease during the subsequent revegetation stage (2016).
Despite this higher sediment supply, they showed that the material delivered
to river systems contained reduced <inline-formula><mml:math id="M149" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs levels compared to the
pre-decontamination period and that this stage of higher sediment supply and
transfer was only temporary due to the rapid vegetation recovery after the
completion of remediation works.</p>
      <p id="d1e2082">The Hagibis super typhoon, which made landfall in Japan on 12 October 2019
(Irasawa et al., 2020), was the first extreme rainfall event that
occurred in the region after the completion of decontamination in the
Special Decontamination Zone early in 2019. Its impact on sediment sources
and sediment <inline-formula><mml:math id="M150" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs contamination was investigated through the analysis
of flood sediment deposits collected in the Mano and Niida river catchments
and through comparison of their geochemical and colour properties with those
analysed in potential sources (e.g. cropland, forests, and subsurface
material originating from landslides and channel bank erosion; Evrard et al., 2020). The results showed that cropland and forests
provided the main supply of sediment and that these sources had reduced
<inline-formula><mml:math id="M151" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations, which may be explained by the effective
decontamination of cropland and the dominance of rill and gully erosion
under forests – mobilising deeper soil layers depleted in <inline-formula><mml:math id="M152" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs –
after such an intense event.</p>
      <p id="d1e2112">A potential concern was that sediment from forests with high <inline-formula><mml:math id="M153" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations (as these zones have not been remediated) may be
transported by river systems and deposited in
nearby remediated cropland due to river overflow during
intense hydrological events, potentially leading to recontamination of these areas.
To investigate this potential issue, sediment that had deposited after the
flood generated by the<?pagebreak page490?> 2019 Hagibis super typhoon was collected along two rivers
in Iitate Village to determine total and exchangeable <inline-formula><mml:math id="M154" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs and
acid-extractable potassium (K) contents (Asano et al., 2022). These
parameters were compared to those measured in nearby decontaminated soils
(where no flood sediment deposition had occurred). Although sediment
deposited by the flood showed 4-times higher <inline-formula><mml:math id="M155" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations than
decontaminated soils, it showed 3-times lower <inline-formula><mml:math id="M156" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs exchangeable
content. Furthermore, acid-extractable K, referred to as non-exchangeable K,
was found to be sufficiently high to restrict <inline-formula><mml:math id="M157" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs transfer from soil
to crops that may be planted in these fields afterwards.</p>
      <p id="d1e2160">Another issue may be related to the intermittent storage of <inline-formula><mml:math id="M158" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
contaminated sediment in the river floodplain, which may be remobilised in the
future during extreme flooding events, although their residence times remain
uncertain (Golosov et al., 2022). This will depend on the
floodplain morphology, vegetation characteristics and on the planning of
management operations (as river channels may be dredged and cleaned by the
authorities). Overall, another study (2015–2019) conducted to determine
changes in radioactive air dose rates in two riverside parks (along
Mizunashi River) of Minamisoma City showed a general decrease in these
rates. They attributed 35 % of the reduction to the physical decay of
radiocesium, 14 % to the vertical migration of radiocesium into the soil
and 51 % to the combined effect of typhoons and remediation works between
2015 and 2019. They additionally outlined the great attenuation of air dose
rates due to the Hagibis super typhoon in 2019, which generated a
significant flush of contaminated sediment stored in the plain towards the
Pacific Ocean (Yamasaki et al., 2023).</p>
      <p id="d1e2172">As fishing was a major recreational activity in the region (which is allowed
after purchasing a fishing ticket from a cooperative), the emergency
monitoring of wild and cultured freshwater products by Fukushima
Prefecture was implemented as soon as on 30 March 2011, with the exception
of the designated evacuation zone (now referred to as the
Difficult-to-Return Zone), which had not been targeted by monitoring
inspections because of the expected high <inline-formula><mml:math id="M159" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activities in freshwater
products (Wada et al., 2022). For cultured fish in ponds (mainly
common carp, salmon and char), very few samples exceeded the Japanese
regulatory limit of 100 Bq kg<inline-formula><mml:math id="M160" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> of <inline-formula><mml:math id="M161" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in 2011–2012, and these
concentrations were found to be below the detection limits of <inline-formula><mml:math id="M162" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
(<inline-formula><mml:math id="M163" display="inline"><mml:mo lspace="0mm">∼</mml:mo></mml:math></inline-formula> 7 Bq kg<inline-formula><mml:math id="M164" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) in all samples from 2015 onwards. This may
be explained by the fact that radiocesium uptake from food was controlled
(using non-contaminated pellets and setting up an intake screen preventing
contaminated wild prey from entering from outside the ponds). In contrast,
several freshwater fishes were contaminated (containing more than 500 Bq kg<inline-formula><mml:math id="M165" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> of radiocesium and up to 18 700 Bq kg<inline-formula><mml:math id="M166" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in 2011–2012); the 100 Bq kg<inline-formula><mml:math id="M167" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> regulatory limit was no longer exceeded in freshwater
fish by 2020 onwards (with the exception of the Difficult-to-Return Zone as
it was not covered by the monitoring inspections). This justified the
prohibition of shipment of eight species (ayu, common carp, crucian carp,
Japanese dace, masu salmon, white-spotted charr, Japanese eel, Japanese
mitten crab) from some areas of Fukushima and four neighbouring
prefectures as of April 2021 and the ongoing prohibition of fishing in the
Difficult-to-Return Zone (where salmon and char fishes showing contamination
levels of up to 25 006 Bq kg<inline-formula><mml:math id="M168" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> were analysed in 2016; Wada et al.,
2019). Although fishing has been allowed again in Abukuma River for most
species as of April 2021, reputational damage remains problematic for the
carp aquaculture industry in particular. For wild species, one of the main
issues in the contamination of salmonids eating prey that consume litter and fungi from contaminated forests, thereby demonstrating
radiocesium accumulation along the food web (Wada et al., 2019).</p>

      <?xmltex \floatpos{t}?><fig id="Ch1.F5"><?xmltex \currentcnt{5}?><?xmltex \def\figurename{Figure}?><label>Figure 5</label><caption><p id="d1e2284">Main dam reservoirs in the radioactive pollution plume of
Fukushima Prefecture.</p></caption>
        <?xmltex \igopts{width=241.848425pt}?><graphic xlink:href="https://soil.copernicus.org/articles/9/479/2023/soil-9-479-2023-f05.png"/>

      </fig>

</sec>
<sec id="Ch1.S9">
  <label>9</label><title>Remobilisation of radionuclides from reservoir and pond sediment</title>
      <p id="d1e2301">Dam reservoirs were shown to act as a sink for radionuclides, where they have
been accumulating for more than 1 decade since the FDNPP accident
(Sakai et al., 2021). In addition to the problems associated with the
accumulation of contaminated sediment in these reservoirs, concerns were
raised regarding the possible remobilisation of radionuclides from the sediment
to the water column under anaerobic conditions. Dissolved <inline-formula><mml:math id="M169" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
concentrations found in sediment-pore<?pagebreak page491?> water from two highly contaminated
reservoirs (i.e. Ogaki Dam and Yokokawa Dam) of the Fukushima-impacted area
(3–66 Bq L<inline-formula><mml:math id="M170" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) were 1 to 2 orders of magnitude higher than in
reservoir water, showing evidence of the remobilisation of bioavailable
<inline-formula><mml:math id="M171" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from sediment (Funaki et al.,
2021). Furthermore, these authors identified a competitive ion exchange
process between <inline-formula><mml:math id="M172" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs and NH<inline-formula><mml:math id="M173" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> via a highly selective
interaction with the frayed edge sites of phyllosilicate minerals, leading
to very high variability of solid–liquid partition coefficient (K<inline-formula><mml:math id="M174" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:math></inline-formula>)
values of sediment-pore water. The continuous supply of <inline-formula><mml:math id="M175" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs-contaminated sediment from the upper catchment prevailed over the diffusive
flux of <inline-formula><mml:math id="M176" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from sediment to overlying water.</p>
      <p id="d1e2383">Accordingly, reservoirs used for irrigation were shown to provide a
perennial source of <inline-formula><mml:math id="M177" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs both in particle-bound and dissolved forms,
in response to resuspension and desorption processes. Furthermore, a control
was identified between reservoir outflow water temperature and dissolved
<inline-formula><mml:math id="M178" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activities in water. This further demonstrated that desorption of
<inline-formula><mml:math id="M179" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from sediment is due to the exchange with cations such as
NH<inline-formula><mml:math id="M180" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> generated by biological activities. Furthermore, dissolved
<inline-formula><mml:math id="M181" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in outflow water exhibited seasonal variations,
with an increasing trend in summer (Kubota et al., 2022).</p>
      <p id="d1e2434">Funaki et al. (2020) investigated <inline-formula><mml:math id="M182" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations in input and
output water from Ogaki Dam Reservoir (2014–2019), and they demonstrated
that dissolved <inline-formula><mml:math id="M183" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations were significantly higher in
outflow than in inflow water. They also calculated the mass balance of
<inline-formula><mml:math id="M184" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in the reservoir and showed that dissolved <inline-formula><mml:math id="M185" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs outputs
were significantly higher than the inputs, and they estimated that
32 %–40 % of the dissolved <inline-formula><mml:math id="M186" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs in the output water was produced
in the reservoir. It therefore represents a source of bioavailable dissolved
<inline-formula><mml:math id="M187" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs, with 0.04–0.09 % of the <inline-formula><mml:math id="M188" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs accumulated in the
reservoir sediment being eluted to the overlaying water each year. Similar
results have been obtained from another reservoir (i.e. Matsugabou Dam) of
Fukushima Prefecture (Hayashi and Tsuji, 2020).</p>
      <p id="d1e2501">Furthermore, in the ponds of Okuma Town from 2015 to 2019 (Konoplev et
al., 2021; Wakiyama et al., 2019), a decline in both particulate and
dissolved <inline-formula><mml:math id="M189" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activity concentrations was revealed. The decline rate
constants for the particulate <inline-formula><mml:math id="M190" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activity concentration were found
to be higher than for the dissolved <inline-formula><mml:math id="M191" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activity concentration. In
terms of seasonality, the dissolved <inline-formula><mml:math id="M192" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs concentrations were higher
from June to October, depending on the specific pond and year, most likely
due to temperature dependence of <inline-formula><mml:math id="M193" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs desorption from frayed edge
sites of micaceous clay minerals. The apparent K<inline-formula><mml:math id="M194" display="inline"><mml:msub><mml:mi/><mml:mi mathvariant="normal">d</mml:mi></mml:msub></mml:math></inline-formula> (<inline-formula><mml:math id="M195" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs) in the
suspended sediment water system was observed to have decreased over time. It was
hypothesised that this trend was associated with the decomposition of glassy
hot particles.</p>
      <p id="d1e2569">This outlines questions regarding the interest of removing contaminated
sediment accumulated in reservoirs in order to limit <inline-formula><mml:math id="M196" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs desorption
and allow the safe resumption of agricultural water use. Another problem is
related to the contamination of fish living in these ponds, as <inline-formula><mml:math id="M197" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
levels analysed in fish collected in 2015–2016 in four ponds in the DTRZ
near the FDNPP were found to be higher than in forest rivers of the zone, and
they systematically exceeded the Japanese regulatory limit (100 Bq kg<inline-formula><mml:math id="M198" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>) by 1 to 3 orders of magnitude (up to
15 700 Bq kg<inline-formula><mml:math id="M199" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula>). This
further demonstrates radiocesium bioaccumulation through the food web around
bottom sediment in the ponds (Wada et al., 2019). This biomagnification
process was observed in lakes and not in rivers (Ishii et al., 2020a).
Even outside of the DTRZ and 5 years later, by 2020, despite remaining below
the 100 Bq kg<inline-formula><mml:math id="M200" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> value, <inline-formula><mml:math id="M201" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs continued to exceed the detection
limits of ca. 7 Bq kg<inline-formula><mml:math id="M202" display="inline"><mml:msup><mml:mi/><mml:mrow><mml:mo>-</mml:mo><mml:mn mathvariant="normal">1</mml:mn></mml:mrow></mml:msup></mml:math></inline-formula> in 92.7 % of fish samples collected from
lakes and ponds of Fukushima Prefecture, where radiocesium has
accumulated and may progressively elute from sediment (Wada et
al., 2022). A peak in <inline-formula><mml:math id="M203" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs activities in lake fish was observed in
summer, which may reflect the preferential remobilisation of <inline-formula><mml:math id="M204" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs from
sediment during this season due to the higher concentrations of
NH<inline-formula><mml:math id="M205" display="inline"><mml:mrow><mml:msubsup><mml:mi/><mml:mn mathvariant="normal">4</mml:mn><mml:mo>+</mml:mo></mml:msubsup></mml:mrow></mml:math></inline-formula> observed in bottom waters, although it may also be attributed
to the higher feeding rates of fish observed during this part of the year
(Matsuzaki et al., 2021).</p>
</sec>
<sec id="Ch1.S10" sec-type="conclusions">
  <label>10</label><title>Conclusions</title>
      <p id="d1e2686">Twelve years after the FDNPP accident, unprecedented soil decontamination
works have been completed across a wide area in Japan and their effectiveness
can be demonstrated through continuous research and monitoring efforts
implemented by numerous Japanese research groups and their foreign
counterparts. Nevertheless, it remains important to continue environmental
monitoring activities initiated after the accident using optimised
spatio-temporal approaches and novel indicators if necessary. Of note, data
collection started earlier after the FDNPP accident compared to the
situation in Chernobyl, and data were more comprehensive and shared in a more
open way in Japan (Hashimoto et al., 2022d; Ishii et al., 2020b; Hashimoto
et al., 2020b), although further improvements remain possible.</p>
      <p id="d1e2689">Based on this post-accidental experience, feedback can be provided to a wide
range of communities to improve our preparedness in potentially affected
regions (e.g. those located in the vicinity of nuclear power plants or
those that may be affected by contaminant deposition following other
industrial accidents) in the future (Hashimoto et al., 2022d). For
instance, to be effective, the removal of the organic matter layer in
deciduous forests should be conducted rapidly after the accident, which is
now too late in the case of Fukushima. As the forest cover is too large to
be fully decontaminated, in addition to the 20 m buffer zones along the
forest edges, priority could be given to the decontamination of the
so-called <italic>satoyama</italic> zones (Hashimoto et al., 2022d). In all cases, providing
added value to the contaminated forest biomass<?pagebreak page492?> is a real issue and it still
requires the further development and consolidation of various economic and
technological approaches.</p>
      <p id="d1e2695">Runoff and river systems were shown to provide significant pathways of
radiocesium redistribution. Accordingly, the expected increased frequency of
typhoons may be of concern, as these events may lead to widespread flooding
and significant forest disturbance (i.e. tree fall and associated
landslides; Morimoto et al., 2021) and associated <inline-formula><mml:math id="M206" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs
transfer. The potential impact of forest fires that may occur more
frequently in the Fukushima region in response to increasing fuel load and
global change should also be investigated as they may lead to the release
of <inline-formula><mml:math id="M207" display="inline"><mml:msup><mml:mi/><mml:mn mathvariant="normal">137</mml:mn></mml:msup></mml:math></inline-formula>Cs into the local atmosphere, as investigated in the
region affected by Chernobyl (Evangeliou et al., 2014). Finally, the spatial
pattern of deposition and subsequent redistribution of microparticles
containing radiocesium that were found in different environmental
compartments, including soils, and that may lead to specific health risks if
they are inhaled should also be further investigated (Fueda et al.,
2023).</p>
</sec>

      
      </body>
    <back><notes notes-type="dataavailability"><title>Data availability</title>

      <p id="d1e2721">All the data provided in this review article can be accessed directly in the
referenced publications or URL. Spatial layers displayed in the figures of this article are freely available on Zenodo (Evrard et
al., 2023).</p>
  </notes><notes notes-type="authorcontribution"><title>Author contributions</title>

      <p id="d1e2727">OE took the initiative and the lead to write this review
article. TCC drew the maps and improved earlier map
versions prepared by OE. TCC, PAC, YW and YT revised and
contributed to the text.</p>
  </notes><notes notes-type="competinginterests"><title>Competing interests</title>

      <p id="d1e2733">At least one of the (co-)authors is a member of the editorial board of <inline-formula><mml:math id="M208" display="inline"><mml:mrow><mml:mi>S</mml:mi><mml:mi>O</mml:mi><mml:mi>I</mml:mi><mml:mi>L</mml:mi></mml:mrow></mml:math></inline-formula>. The peer-review process was guided by an independent editor, and the authors also have no other competing interests to declare.</p>
  </notes><notes notes-type="disclaimer"><title>Disclaimer</title>

      <p id="d1e2753">Publisher’s note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.</p>
  </notes><ack><title>Acknowledgements</title><p id="d1e2759">The support of CNRS (Centre National de la Recherche Scientifique, France),
CEA (Commissariat à l'Energie Atomique et aux Energies Alternatives,
France) and the Institute of Environmental Radioactivity (IER) of Fukushima University in the framework of the MITATE Lab International Research Project (IRP) is gratefully acknowledged.</p></ack><notes notes-type="financialsupport"><title>Financial support</title>

      <p id="d1e2764">This research benefitted from the support of the AMORAD (grant no. ANR-11-RSNR-0002)
project (ANR, Agence Nationale de la Recherche, Programme des
Investissements d'Avenir). This work was also supported by ERAN
(Environmental Radioactivity Research Network Center), grant nos. I-21-22 and
I-22-24. Thomas Chalaux-Clergue obtained a PhD fellowship from CEA, France,
and a JSPS grant, which supported spending of the second PhD year at Kyoto Prefectural
University (October 2022–September 2023). This work was also supported by
Grants-in-Aid for JSPS Fellows (Pierre-Alexis Chaboche, grant no. 22F22712;
Thomas Chalaux-Clergue, grant no. PE22708).</p>
  </notes><notes notes-type="reviewstatement"><title>Review statement</title>

      <p id="d1e2770">This paper was edited by Rafael Clemente and reviewed by two anonymous referees.</p>
  </notes><ref-list>
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