Following the Fukushima Daiichi Nuclear Power Plant disaster in March 2011, the Japanese government initiated an unprecedented decontamination programme to remediate 137Cs-contaminated soils and allow population return. This programme involved the removal of topsoil under farmland and residential land, and its replacement with \"fresh soil\" composed of granitic saprolite. However, decontamination was limited to these two land uses, without remediating forests, which cover 70 % of the surface area in the affected region. In this unprecedented context, the specific impact of this unique decontamination programme on 137Cs transfers in river systems remains to be quantified at the catchment scale. In this study, based on the analysis of a sediment core collected in June 2021 in the Mano Dam reservoir draining a decontaminated catchment, the effects of soil decontamination on particle-bound 137Cs dynamics and sediment source contributions in response to a succession of extreme precipitation events were retrospectively assessed. The sequence of sediment layer deposition and its chronology were reconstructed through the analysis of several diagnostic properties (organic matter, elemental geochemistry, visible colourimetry, granulometry) and contextual information. During abandonment (2011-2016), cropland contribution decreased (31 %). Concurrently, 137Cs activity and deposition flux decreased (19 and 29%year-1, respectively). Following decontamination (2017), sediment transfer increased (270 %) in response to increased contributions from decontaminated cropland and \"fresh soil\" (625 % and 180 % respectively). Meanwhile, forest contributions remained stable. In contrast, 137Cs activity dropped (65 %), although 137Cs deposition flux remained constant. Forests acted as a stable source of 137Cs. Accordingly, 137Cs deposition flux after decontamination (2016-2021) was similar to that observed during the 5-years period of land abandonment (2011-2016), as a result of the regrowth of spontaneous vegetation over farmland, protecting soil against erosion. Future research should further investigate the impact of longer land abandonment that prevailed in some regions decontaminated lately on the 137Cs fluxes in the rivers.

Sediment source fingerprinting has been progressively developed and refined over the past 40 years or more and now represents a widely used and valuable technique, with important practical applications. However, relatively little attention has been given to the target samples and the extent to which they are able to provide meaningful information on short- or longer-term relative source contributions for a given study catchment. A key issue here is the inherent short- and longer-term temporal variability of source contributions and the extent to which such variability is taken into account by the target samples. The objective of this study was to investigate the temporal variation of source contributions from the Qiaozi West catchment, a small (1.09 km2) gully catchment located within the Loess Plateau of China. The target samples represented a suite of 214 spot suspended sediment samples collected during eight representative wet season rainfall events occurring over two years. A suite of geochemical properties was used as fingerprints and standard source apportionment calculations indicated that the gully walls contributed the most sediment (load-weighted mean 54.5%) and, together with cropland (load-weighted mean 37.3%), and gully slopes (load-weighed mean 6.6%) were the main sediment sources. The 214 individual target samples indicated that the contribution of cropland sources varied between 8.3% and 60.4%, gully walls between 22.9% and 85.8% and gully slopes between 1.1% and 30.7%, representing ranges of 52.1%, 62.9% and 29.6% respectively. In order to explore whether the temporal variability of source contributions demonstrated by the study catchment should be seen as typical, equivalent information was abstracted from 14 published studies for other catchments of varying size and located in different environments worldwide. This information demonstrated similar temporal variability of the relative contributions of the major sources, which were typically characterized by ranges of the order of 30-70%. The temporal variability associated with the estimates of relative source contributions provided by target samples has important implications for the uncertainty associated with such estimates derived using source fingerprinting techniques based on a limited number of target samples. Further attention needs to be directed to the design of sampling programmes used to collect such samples and to taking account of such uncertainty in source apportionment calculations.

Excessive sediment loss degrades freshwater quality and is prone to further elevation and variable source contributions due to the combined effect of extreme rainfall and differing land uses. To quantify erosion and sediment source responses across scales, this study integrated work at both field and catchment scale for two hydrologically contrasting winters (2018-19 and 2019-20). Sediment load was estimated at the field scale (grassland-arable conversion system). Sediment source apportionment work was undertaken at the catchment scale (4.5 km2) and used alkanes, and both free and bound fatty acid carbon isotope signatures as diagnostic fingerprints to distinguish sediment sources: arable, pasture, woodland and stream banks. Sediment source apportionment based on bound fatty acids revealed a substantial shift in contributions, from stream banks dominating (70 ± 5%) in winter 2018-19, to arable land dominating (52 ± 7%) in the extreme wet winter 2019-20. Increases in sediment contributions from arable (∼3.9 times) and pasture (∼2.4 times) land at the catchment outlet during the winter 2019-20 were consistent with elevated sediment losses monitored at the field scale which indicated that low-magnitude high frequency rainfall alone increased sediment loss even from pasture by 350%. In contrast, carbon isotope signatures of alkanes and free fatty acids consistently estimated stream banks as a dominant source (i.e., ∼36% and ∼70% respectively) for both winters regardless of prolonged rainfall in winter 2019-20. Beyond quantifying the shifts in field scale sediment load and catchment scale sediment sources due to the changes in rainfall patterns, our results demonstrate valuable insight into how the fate of biotracers in soil and sediment manifests in the δ13C values of homologues and, in turn, their role in information gain for estimating sediment source contributions. Discrepancies in the estimated sediment source contributions using different biotracers indicate that without a careful appreciation of their biogeochemical limitations, erroneous interpretation of sediment source contributions can undermine management strategies for delivering more sustainable and resilient agriculture.

A Compound Specific Stable Isotope (CSSI) sediment tracing approach is applied for the first time in a Mediterranean mountain agroforestry catchment subjected to intense land use changes in the past decades. Many Mediterranean mountain environments underwent conversion of rangelands into croplands during the previous centuries to increase agricultural production. Converted land has increased the risk of erosion and in some cases has led to loss of the entire fertile topsoil. After land abandonment the process was gradually reversed during the middle of the 20th century, allowing the recovery of natural land cover and reduction of soil erosion rates. The 13C abundance of long chain fatty acids was used as tracer to assess the contribution of soil under different vegetation covers in complex landscapes subjected to land use changes after land abandonment in a medium-sized Mediterranean catchment. A Bayesian mixing model (MixSIAR) was used for estimating the contribution of different land use types to suspended sediments. To this purpose, composite samples were collected over the four main land covers existing in the study area: cropland, Mediterranean forest, pine forest, scrubland, and two main geomorphic elements: highly disturbed areas such as exposed subsoil and channel banks. Suspended sediment traps were installed at three locations in the catchment to assess the variability of source contributions from the headwaters to the outlet of the catchment. At every sampling point three replicating traps integrated the suspended sediment per climatologic season during a one hydrological year. The fatty acids (FAs) content was significantly higher at the catchment outlet than at the headwaters. The δ13C signatures of the FAs were successful in discriminating between Mediterranean forest, scrubland, pine forest and both geomorphic elements. Overall, the model identified agricultural land as the largest contributing source for most of the sampled seasons. The inclusion of prior information with different informativeness produced variations in the model outputs and could represent an advantage as much as a disadvantage if priors are not used with caution and supported by robust evidence. The results of this study suggest that CSSI tracers are needed to correctly assess land use related sediment sources, while channel bank and subsoil contributions require geochemical tracers. The high agricultural apportionment despite its small coverage (16%) point out to the impact of human activities and the agriculture cycle on soil loss in these mountain agroforestry systems.

Sediment source fingerprinting has been successfully deployed to provide information on the surface and subsurface sources of sediment in many catchments around the world. However, there is still scope to re-examine some of the major assumptions of the technique with reference to the number of fingerprint properties used in the model, the number of model iterations and the potential uncertainties of using more than one sediment core collected from the same floodplain sink. We investigated the role of subsurface erosion in the supply of fine sediment to two sediment cores collected from a floodplain in a small degraded catchment in the Eastern Cape, South Africa. The results showed that increasing the number of individual fingerprint properties in the composite signature did not improve the model goodness-of-fit. This is still a much debated issue in sediment source fingerprinting. To test the goodness-of-fit further, the number of model repeat iterations was increased from 5000 to 30,000. However, this did not reduce uncertainty ranges in modelled source proportions nor improve the model goodness-of-fit. The estimated sediment source contributions were not consistent with the available published data on erosion processes in the study catchment. The temporal pattern of sediment source contributions predicted for the two sediment cores was very different despite the cores being collected in close proximity from the same floodplain. This highlights some of the potential limitations associated with using floodplain cores to reconstruct catchment erosion processes and associated sediment source contributions. For the source tracing approach in general, the findings here suggest the need for further investigations into uncertainties related to the number of fingerprint properties included in un-mixing models. The findings support the current widespread use of ≤5000 model repeat iterations for estimating the key sources of sediment samples.

Fine sediment inputs into river systems can be a major source of nutrients and heavy metals and have a strong impact on water quality and ecosystem functions of rivers and lakes, including those in semiarid regions. However, little is known to date about the spatial distribution of sediment sources in most large scale river basins in Central Asia. Accordingly, a sediment source fingerprinting technique was used to assess the spatial sources of fine-grained (<10 μm) sediment in the 15 000 km(2) Kharaa River basin in northern Mongolia. Variation in geochemical composition (e.g. in Ti, Sn, Mo, Mn, As, Sr, B, U, Ca and Sb) was used for sediment source discrimination with geochemical composite fingerprints based on Genetic Algorithm (GA)-driven Discriminant Function Analysis, the Kruskal-Wallis H-test and Principal Component Analysis. All composite fingerprints yielded a satisfactory GOF (>0.97) and were subsequently used for numerical mass balance modelling with uncertainty analysis. The contributions of the individual sub-catchment spatial sediment sources varied from 6.4% (the headwater sub-catchment of Sugnugur Gol) to 36.2% (the Kharaa II sub-catchment in the middle reaches of the study basin), generally showing higher contributions from the sub-catchments in the middle, rather than the upstream, portions of the study area. The importance of river bank erosion is shown to increase from upstream to midstream tributaries. The source tracing procedure provides results in reasonable accordance with previous findings in the study region and demonstrates the applicability and associated uncertainties of the approach for fine-grained sediment source investigation in large scale semi-arid catchments.

There is increasing global concern regarding the impacts of large scale land disturbance by wildfire on a wide range of water and related ecological services. This study explores the impact of the 2003 Lost Creek wildfire in the Crowsnest River basin, Alberta, Canada on regional scale sediment sources using a tracing approach. A composite geochemical fingerprinting procedure was used to apportion the sediment efflux among three key spatial sediment sources: 1) unburned (reference) 2) burned and 3) burned sub-basins that were subsequently salvage logged. Spatial sediment sources were characterized by collecting time-integrated suspended sediment samples using passive devices during the entire ice free periods in 2009 and 2010. The tracing procedure combines the Kruskal-Wallis H-test, principal component analysis and genetic-algorithm driven discriminant function analysis for source discrimination. Source apportionment was based on a numerical mass balance model deployed within a Monte Carlo framework incorporating both local optimization and global (genetic algorithm) optimization. The mean relative frequency-weighted average median inputs from the three spatial source units were estimated to be 17% (inter-quartile uncertainty range 0-32%) from the reference areas, 45% (inter-quartile uncertainty range 25-65%) from the burned areas and 38% (inter-quartile uncertainty range 14-59%) from the burned-salvage logged areas. High sediment inputs from burned and the burned-salvage logged areas, representing spatial source units 2 and 3, reflect the lasting effects of forest canopy and forest floor organic matter disturbance during the 2003 wildfire including increased runoff and sediment availability related to high terrestrial erosion, streamside mass wasting and river bank collapse. The results demonstrate the impact of wildfire and incremental pressures associated with salvage logging on catchment spatial sediment sources in higher elevation Montane regions where forest growth and vegetation recovery are relatively slow.