Drivers and human impacts on topsoil bacterial and fungal community biogeography across Australia.

Soil microbial diversity mediates a wide range of key processes and ecosystem services influencing planetary health. Our knowledge of microbial biogeography patterns, spatial drivers and human impacts at the continental scale remains limited. Here, we reveal the drivers of bacterial and fungal community distribution in Australian topsoils using 1384 soil samples from diverse bioregions. Our findings highlight that climate factors, particularly precipitation and temperature, along with soil properties, are the primary drivers of topsoil microbial biogeography. Using random forest machine-learning models, we generated high-resolution maps of soil bacteria and fungi across continental Australia. The maps revealed microbial hotspots, for example, the eastern coast, southeastern coast, and west coast were dominated by Proteobacteria and Acidobacteria. Fungal distribution is strongly influenced by precipitation, with Ascomycota dominating the central region. This study also demonstrated the impact of human modification on the underground microbial community at the continental scale, which significantly increased the relative abundance of Proteobacteria and Ascomycota, but decreased Chloroflexi and Basidiomycota. The variations in microbial phyla could be attributed to distinct responses to altered environmental factors after human modifications. This study provides insights into the biogeography of soil microbiota, valuable for regional soil biodiversity assessments and monitoring microbial responses to global changes.

A robust interpolation-based method for forensic soil provenancing: A Bayesian likelihood ratio approach.

Soil is a complex and spatially variable material that has a demonstrated potential as a useful evidence class in forensic casework and intelligence operations. Here, the capability to spatially constrain police search areas and prioritise resources by triaging areas as low and high interest is advantageous. Conducted between 2017 and 2021, a forensically relevant topsoil survey (0-5 cm depth; 1 sample per 1 km2) was carried out over Canberra, Australia, aiming to document the distribution of chemical elements in an urban/suburban environment, and of acting as a testbed for investigating various aspects of forensic soil provenancing. Geochemical data from X-Ray Fluorescence (XRF; for total major oxides) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS; for trace elements) following a total digestion (HF + HNO3) of the fused XRF beads were obtained from the survey's 685 topsoil samples (plus 138 additional quality control samples and six "Blind" simulated evidentiary samples). Using those "Blind" samples, we document a likelihood ratio approach where for each grid cell the analytical similarity between the grid cell and evidentiary sample is attributed from a measure of overlap between the two Cauchy distributions, including appropriate uncertainties. Unlike existing methods that base inclusion/exclusion on an arbitrary threshold (e.g., ± three standard deviations), our approach is free from strict binary or Boolean thresholds, providing an unconstrained gradual transition dictated by the analytical similarity. Using this provenancing model, we present and evaluate a new method for upscaling from a fine (25 m x 25 m) interpolated grid to a more appropriate coarser (500 m x 500 m) grid. In addition, an objective method using Random Match Probabilities for ranking individual variables to be used for provenancing prior to receiving evidentiary material was demonstrated. Our results show this collective procedure generates more consistent and robust provenance maps when applied to two different interpolation algorithms (e.g., inverse distance weighting, and natural neighbour), with different grid placements (e.g., grid shifts to the north or east) and by different theoretical users (e.g., different computer systems, or forensic geoscientists).

The secret hidden in dust: Assessing the potential to use biological and chemical properties of the airborne fraction of soil for provenance assignment and forensic casework.

The airborne fraction of soil (dust) is both ubiquitous in nature and contains localised biological and chemical signatures, making it a potential medium for forensic intelligence. Metabarcoding of dust can yield biological communities unique to the site of interest, similarly, geochemical analyses can uncover elements and minerals within dust that can be matched to a geographic location. Combining these analyses presents multiple lines of evidence as to the origin of dust collected from items of interest. In this work, we investigated whether bacterial and fungal communities in dust change through time and whether they are comparable to soil samples of the same site. We integrated dust metabarcoding into a framework amenable to forensic casework, (i.e., using calibrated log-likelihood ratios) to predict the origin of dust samples using models constructed from both dust samples and soil samples from the same site. Furthermore, we tested whether both metabarcoding and geochemical/mineralogical analyses could be conducted on a single swabbed sample, for situations where sampling is limited. We found both analyses could generate results from a single swabbed sample and found biological and chemical signatures unique to sites. However, we did find significant variation within sites, where this did not always correlate with time but was a random effect of sampling. This variation within sites was not greater than between sites and so did not influence site discrimination. When modelling bacterial and fungal diversity using calibrated log-likelihood ratios, we found samples were correctly predicted using dust 67% and 56% of the time and using soil 56% and 22% of the time for bacteria and fungi communities respectively. Incorrect predictions were related to within site variability, highlighting limitations to assigning dust provenance using metabarcoding of soil.

The utility of dust for forensic intelligence: Exploring collection methods and detection limits for environmental DNA, elemental and mineralogical analyses of dust samples.

Environmental DNA (eDNA), elemental and mineralogical analyses of soil have been shown to be specific to their source material, prompting consideration of using the airborne fraction of soil (dust) for forensic intelligence work. Dust is ubiquitous in the environment and is easily transferred to items belonging to a person of interest, making dust analysis an ideal tool in forensic casework. The advent of Massive Parallel Sequencing technologies means metabarcoding of eDNA can uncover bacterial, fungal, and even plant genetic fingerprints in dust particles. Combining this with elemental and mineralogical compositions offers multiple, complementary lines of evidence for tracing the origin of an unknown dust sample. This is particularly pertinent when recovering dust from a person of interest to ascertain where they may have travelled. Prior to proposing dust as a forensic trace material, however, the optimum sampling protocols and detection limits need to be established to place parameters around its utility in this context. We tested several approaches to collecting dust from different materials and determined the lowest quantity of dust that could be analysed for eDNA, elemental composition and mineralogy, whilst still yielding results capable of distinguishing between sites. We found that fungal eDNA profiles could be obtained from multiple sample types and that tape lifts were the optimum collection method for discriminating between sites. We successfully recovered both fungal and bacterial eDNA profiles down to 3 mg of dust (the lowest tested quantity) and recovered elemental and mineralogical compositions for all tested sample quantities. We show that dust can be reliably recovered from different sample types, using different sampling techniques, and that fungi and bacteria, as well as elemental and mineralogical profiles, can be generated from small sample quantities, highlighting the utility of dust for forensic intelligence.

Forensic soil provenancing in an urban/suburban setting: A simultaneous multivariate approach.

Soil is a ubiquitous material at the Earth's surface with potential to be a useful evidence class in forensic and intelligence applications. Compositional data from a soil survey over North Canberra, Australian Capital Territory, are used to develop and test an empirical soil provenancing method. Mineralogical data from Fourier Transform InfraRed spectroscopy (FTIR) and geochemical data from X-Ray Fluorescence (XRF; for total major oxides) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS; for both total and aqua regia-soluble trace elements) are obtained from the survey's 268 topsoil samples (0-5 cm depth; 1 sample per km2 ). The simultaneous provenancing approach is underpinned by (i) the calculation of Spearman's correlation coefficients (rS ) between an evidentiary sample and all the samples in the database for all variables generated by each analytical method; and (ii) the preparation of an interpolated raster grid of rS for each evidentiary sample and method resulting in a series of provenance rasters ("heat maps"). The simultaneous provenancing method is tested on the North Canberra soil survey with three "blind" samples representing simulated evidentiary samples. Performance metrics of precision and accuracy indicate that the FTIR (mineralogy) and XRF (geochemistry) analytical methods offer the most precise and accurate provenance predictions. Maximizing the number of analytes/analytical techniques is advantageous in soil provenancing. Despite acknowledged limitations, it is concluded that the empirical soil provenancing approach can play an important role in forensic and intelligence applications.

Forensic soil provenancing in an urban/suburban setting: A sequential multivariate approach.

Compositional data from a soil survey over North Canberra, Australian Capital Territory, are used to develop and test an empirical soil provenancing method. Mineralogical data from Fourier transform infrared spectroscopy (FTIR) and magnetic susceptibility (MS), and geochemical data from X-ray fluorescence (XRF; for total major oxides) and inductively coupled plasma-mass spectrometry (ICP-MS; for both total and aqua regia-soluble trace elements) are performed on the survey's 268 topsoil samples (0-5 cm depth; 1 sample per km2 ). Principal components (PCs) are calculated after imputation of censored data and centered log-ratio transformation. The sequential provenancing approach is underpinned by (i) the preparation of interpolated raster grids of the soil properties (including PCs); (ii) the explicit quantification and propagation of uncertainty; (iii) the intersection of the soil property rasters with the values of the evidentiary sample (± uncertainty); and (iv) the computation of cumulative provenance rasters ("heat maps") for the various analytical techniques. The sequential provenancing method is tested on the North Canberra soil survey with three "blind" samples representing simulated evidentiary samples. Performance metrics of precision and accuracy indicate that the FTIR and MS (mineralogy), as well as XRF and total ICP-MS (geochemistry) analytical methods, offer the most precise and accurate provenance predictions. Inclusion of PCs in provenancing adds marginally to the performance. Maximizing the number of analytes/analytical techniques is advantageous in soil provenancing. Despite acknowledged limitations and gaps, it is concluded that the empirical soil provenancing approach can play an important role in forensic and intelligence applications.

Future migration: Key environmental indicators of Pu accumulation in terrestrial sediments of Queensland, Australia.

Plutonium (Pu) interactions in the environment are highly complex. Site-specific variables play an integral role in determining the chemical and physical form of Pu, and its migration, bioavailability, and immobility. This paper aims to identify the key variables that can be used to highlight regions of radioecological sensitivity and guide remediation strategies in Australia. Plutonium is present in the Australian environment as a result of global fallout and the British nuclear testing program of 1952-1958 in central and west Australia (Maralinga and Montebello islands). We report the first systematic measurements of 239+240Pu and 238Pu activity concentrations in distal (≥1000 km from test sites) catchment outlet sediments from Queensland, Australia. The average 239+240Pu activity concentration was 0.29 mBq.g -1 (n = 73 samples) with a maximum of 4.88 mBq.g -1.238Pu/239+240Pu isotope ratios identified a large range (0.02-0.29 (RSD: 74%)) which is congruent with the heterogeneous nuclear material used for the British nuclear testing programme at Maralinga and Montebello Islands. The use of a modified PCA relying on non-linear distance correlation (dCorr) provided broader insight into the impact of environmental variables on the transport and migration of Pu in this soil system. Primary key environmental indicators of Pu presence were determined to be actinide/lanthanide/heavier transition metals, elevation, electrical conductivity (EC), CaO, SiO2, SO3, landform, geomorphology, land use, and climate explaining 81.7% of the variance of the system. Overall this highlighted that trace level Pu accumulations are associated with the coarse, refractive components of Australian soils, and are more likely regulated by the climate of the region and overall soil type.

Predictive Soil Provenancing (PSP): An Innovative Forensic Soil Provenance Analysis Tool.

Soil is a common evidence type used in forensic and intelligence operations. Where soil composition databases are lacking or inadequate, we propose to use publicly available soil attribute rasters to reduce forensic search areas. Soil attribute rasters, which have recently become widely available at high spatial resolutions, typically three arc-seconds (~90 m), are predictive models of the distribution of soil properties (with confidence limits) derived from data mining the inter-relationships between these properties and several environmental covariates. Each soil attribute raster is searched for pixels that satisfy the compositional conditions of the evidentiary soil sample (target value ± confidence limits). We show through an example that the search area for an evidentiary soil sample can be reduced to <10% of the original investigation area. This Predictive Soil Provenancing (PSP) approach is a transparent, reproducible, and objective method of efficiently and effectively reducing the likely provenance area of forensic soil samples.

Quantifying Diffuse Contamination: Method and Application to Pb in Soil.

A new method for detecting and quantifying diffuse contamination at the continental to regional scale is based on the analysis of cumulative distribution functions (CDFs). It uses cumulative probability (CP) plots for spatially representative data sets, preferably containing >1000 determinations. Simulations demonstrate how different types of contamination influence elemental CDFs of different sample media. It is found that diffuse contamination is characterized by a distinctive shift of the low-concentration end of the distribution of the studied element in its CP plot. Diffuse contamination can be detected and quantified via either (1) comparing the distribution of the contaminating element to that of an element with a geochemically comparable behavior but no contamination source (e.g., Pb vs Rb), or (2) comparing the top soil distribution of an element to the distribution of the same element in subsoil samples from the same area, taking soil forming processes into consideration. Both procedures are demonstrated for geochemical soil data sets from Europe, Australia, and the U.S.A. Several different data sets from Europe deliver comparable results at different scales. Diffuse Pb contamination in surface soil is estimated to be <0.5 mg/kg for Australia, 1-3 mg/kg for Europe, and 1-2 mg/kg, or at least <5 mg/kg, for the U.S.A. The analysis presented here also allows recognition of local contamination sources and can be used to efficiently monitor diffuse contamination at the continental to regional scale.

Publicly available datasets on thallium (Tl) in the environment-a comment on "Presence of thallium in the environment: sources of contaminations, distribution and monitoring methods" by Bozena Karbowska, Environ Monit Assess (2016) 188:640 (DOI 10.1007/s10661-016-5647-y).

This comment highlights a whole series of datasets on thallium concentrations in the environment that were overlooked in the recent review by Karbowska, Environmental Monitoring and Assessment, 188, 640, 2016 in this journal. Geochemical surveys carried out over the last few decades all over the world at various scales and using different sampling media have reported the concentration of thallium (and dozens more elements) in tens of thousands of samples. These datasets provide a 'real-world' foundation upon which source apportionment investigations can be based, monitoring programs devised and modelling studies designed. Furthermore, this comment also draws attention to two global geochemical mapping initiatives that should be of interest to environmental scientists.

Establishing geochemical background variation and threshold values for 59 elements in Australian surface soil.

During the National Geochemical Survey of Australia over 1300 top (0-10cm depth) and bottom (~60-80cm depth) sediment samples (including ~10% field duplicates) were collected from the outlet of 1186 catchments covering 81% of the continent at an average sample density of 1 site/5200km2. The <2mm fraction of these samples was analysed for 59 elements by ICP-MS following an aqua regia digestion. Results are used here to establish the geochemical background variation of these elements, including potentially toxic elements (PTEs), in Australian surface soil. Different methods of obtaining geochemical threshold values, which differentiate between background and those samples with unusually high element concentrations and requiring attention, are presented and compared to Western Australia's 'ecological investigation levels' (EILs) established for 14 PTEs. For Mn and V these EILs are so low that an unrealistically large proportion (~24%) of the sampled sites would need investigation in Australia. For the 12 remaining elements (As, Ba, Cd, Co, Cr, Cu, Hg, Mo, Ni, Pb, Sn and Zn) few sample sites require investigation and as most of these are located far from human activity centres, they potentially suggest either minor local contamination or mineral exploration potential rather than pollution. No major diffuse source of contamination by PTEs affects Australian soil at the continental scale. Of the statistical methods used to establish geochemical threshold values, the most pertinent results come from identifying breaks in cumulative probability distributions, the Tukey inner fence and the 98th percentile. Geochemical threshold values for 59 elements, including emerging 'high-tech' critical elements such as lanthanides, Be, Ga or Ge, for which no EILs currently exist, are presented.

Satellite-derived mineral mapping and monitoring of weathering, deposition and erosion.

The Earth's surface comprises minerals diagnostic of weathering, deposition and erosion. The first continental-scale mineral maps generated from an imaging satellite with spectral bands designed to measure clays, quartz and other minerals were released in 2012 for Australia. Here we show how these satellite mineral maps improve our understanding of weathering, erosional and depositional processes in the context of changing weather, climate and tectonics. The clay composition map shows how kaolinite has developed over tectonically stable continental crust in response to deep weathering during northwardly migrating tropical conditions from 45 to 10 Ma. The same clay composition map, in combination with one sensitive to water content, enables the discrimination of illite from montmorillonite clays that typically develop in large depositional environments over thin (sinking) continental crust such as the Lake Eyre Basin. Cutting across these clay patterns are sandy deserts that developed <10 Ma and are well mapped using another satellite product sensitive to the particle size of silicate minerals. This product can also be used to measure temporal gains/losses of surface clay caused by periodic wind erosion (dust) and rainfall inundation (flood) events. The accuracy and information content of these satellite mineral maps are validated using published data.

Pedogeochemistry in NE-Brazil - compared to Australia and Europe.

A soil geochemical dataset (major and minor elements), based on low-density sampling, is provided for NE-Brazil (ca. 1.7 million km²). It covers an area from about 2°S to 12°S, and from 34°W to 49°W, and refers to top (TOP: 0-20 cm) and bottom (BOT: 30-50 cm) mineral soils. Results are put in perspective using two recent and comparable studies, the National Geochemical Survey of Australia (NGSA) and the European Geochemical Mapping of Agricultural Soils (GEMAS). All median element concentrations in the Brazilian samples are depleted compared to World Soil Averages (WSA), except for Al2O3 and SiO2, which are respectively similar to WSA and enriched in Brazil. While the depletion is moderate for Fe2O3, MnO, P2O5, and TiO2, it reaches an order of magnitude and more for K2O, MgO, CaO, and Na2O. The difference between TOP and BOT concentrations is lower than the variation of either TOP or BOT concentrations between sample sites. Similar spatial distribution and the high correlation between TOP and BOT concentrations suggest that (1) similar processes and parameters are of general relevance for the geochemical composition of TOP and BOT samples, and (2) topsoil and subsoil are not decoupled. Cluster analysis revealed similar results for TOP and BOT samples, yielding three groups of elements/oxides displaying similar behavior: Gr.1 comprising Al2O3, Fe2O3, TiO2, and P2O5; Gr.2 comprising CaO, K2O, MgO, MnO, and Na2O; and Gr.3 being SiO2. Weathering indicators are significantly positively correlated and show similar spatial distributions in TOP and BOT samples. All elements deliver similar mass removal times (time to export all material from a 10 cm soil layer) and clearly discern between the regions: Europe with the fastest "depletion" (12,200 ± 300 years), followed by Australia (33,200 ± 3000 years) and Brazil (86,700 ± 3000 years). Similar results emerge when calculating denudation rates, using independent fluvial denudation data in large basins.

Safe storage and effective monitoring of CO2 in depleted gas fields.

Carbon capture and storage (CCS) is vital to reduce CO(2) emissions to the atmosphere, potentially providing 20% of the needed reductions in global emissions. Research and demonstration projects are important to increase scientific understanding of CCS, and making processes and results widely available helps to reduce public concerns, which may otherwise block this technology. The Otway Project has provided verification of the underlying science of CO(2) storage in a depleted gas field, and shows that the support of all stakeholders can be earned and retained. Quantitative verification of long-term storage has been demonstrated. A direct measurement of storage efficiency has been made, confirming that CO(2) storage in depleted gas fields can be safe and effective, and that these structures could store globally significant amounts of CO(2).

New soil composition data for Europe and Australia: demonstrating comparability, identifying continental-scale processes and learning lessons for global geochemical mapping.

New geochemical data from two continental-scale soil surveys in Europe and Australia are compared. Internal project standards were exchanged to assess comparability of analytical results. The total concentration of 26 oxides/elements (Al2O3, As, Ba, CaO, Ce, Co, Cr, Fe2O3, Ga, K2O, MgO, MnO, Na2O, Nb, Ni, P2O5, Pb, Rb, SiO2, Sr, Th, TiO2, V, Y, Zn, and Zr), Loss On Ignition (LOI) and pH are demonstrated to be comparable. Additionally, directly comparable data for 14 elements in an aqua regia extraction (Ag, As, Bi, Cd, Ce, Co, Cs, Cu, Fe, La, Li, Mn, Mo, and Pb) are provided for both continents. Median soil compositions are close, though generally Australian soils are depleted in all elements with the exception of SiO2 and Zr. This is interpreted to reflect the generally longer and, in places, more intense weathering in Australia. Calculation of the Chemical Index of Alteration (CIA) gives a median value of 72% for Australia compared to 60% for Europe. Element concentrations vary over 3 (and up to 5) orders of magnitude. Several elements (total As and Ni; aqua regia As, Co, Bi, Li, Pb) have a lower element concentration by a factor of 2-3 in the soils of northern Europe compared to southern Europe. The break in concentration coincides with the maximum extent of the last glaciation. The younger soils of northern Europe are more similar to the Australian soils than the older soils from southern Europe. In Australia, the central region with especially high SiO2 concentrations is commonly depleted in many elements. The new data define the natural background variation for two continents on both hemispheres based on real data. Judging from the experience of these two continental surveys, it can be concluded that analytical quality is the key requirement for the success of global geochemical mapping.

Distinguishing between natural and anthropogenic sources for elements in the environment: regional geochemical surveys versus enrichment factors.

High element enrichment factors (EFs) are commonly used in the literature to support the hypothesis that a particular suite of elements is of anthropogenic origin. Real-world examples of regional geochemical surveys demonstrate that EFs can be high or low due to a multitude of reasons, of which contamination is but one. This applies to EFs calculated relative to either the crust or some local background (e.g., a deeper soil layer). Results from local studies near industrial centres showing high (and pollution-related) EFs cannot be generalised over large areas or for sample sites far removed (i.e., more than some tens of kilometers) from a likely pollution source. Regional-scale geochemical mapping, on the other hand, facilitates the reliable estimation of the influence of contamination on the measured element concentrations. EFs are strongly influenced by, among other factors, biogeochemical processes that redistribute chemical elements between environmental compartments at the Earth's surface. Using EFs to detect or 'prove' human influence on element cycles in remote areas should be avoided because, in most cases, high EFs cannot conclusively demonstrate, nor even suggest, such influence.

Chemical composition of arctic snow: concentration levels and regional distribution of major elements.

At the end of the northern winter 1996/1997, 21 snow samples were collected from 17 arctic localities in Norway, Sweden, Finland, Svalbard, Russia, Alaska, Canada, Greenland and Iceland. Major element concentrations of the filtered (0.45 mum) melted snow indicate that most samples are consistent with a diluted seawater composition. Deviations from this behaviour indicate additional SO(4)(2-) and Cl(-) relative to seawater, suggesting a minor contribution from (probably local) coal combustion emissions (Alaska, Finland, Sweden, Svalbard). The samples with the highest Na and Cl(-) content (Canada, Russia) also have higher Na/SO(4)(2-) and Cl(-)/SO(4)(2-) ratios than seawater, suggesting a slight contamination from (probably local) deicing activities. Local soil or rock dust inputs in the snow are indicated by 'excess' Ca contents (Alaska, Svalbard, Greenland, Sweden). No overall relationship was found between pH (range: 4.6-6.1) and total or non-seasalt SO(4)(2-) (NSS), suggesting that acidification due to long-range transport of SO(2) pollution is not operating on an arctic-wide scale. In a few samples (Alaska, Finland, Sweden, Svalbard), a significant proportion (>50%) of SO(4)(2-) is non-marine in origin. Sources for this non-marine SO(4)(2-) need not all be found in long-range atmospheric transport and more likely sources are local industry (Finland, Sweden), road traffic (Alaska) or minor snow-scooting traffic (one Svalbard locality). A few samples from northern Europe show a relatively weak trend of decreasing pH with increasing NO(3)(-).