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At least 1,369 records · Page 76

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DOE OSTI2020

A spatial emergent constraint on the sensitivity of soil carbon turnover to global warming

Carbon cycle feedbacks represent large uncertainties in climate change projections, and the response of soil carbon to climate change contributes the greatest uncertainty to this. Future changes in soil carbon depend on changes in litter and root inputs from plants and especially on reductions in the turnover time of soil carbon (τ s ) with warming. An approximation to the latter term for the top one metre of soil (ΔC s,τ ) can be diagnosed from projections made with the CMIP6 and CMIP5 Earth System Models (ESMs), and is found to span a large range even at 2 °C of global warming (-196 ± 117 PgC). Here, we present a constraint on ΔC s,τ , which makes use of current heterotrophic respiration and the spatial variability of τs inferred from observations. This spatial emergent constraint allows us to halve the uncertainty in ΔC s,τ at 2 °C to -232 ± 52 PgC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Moiré-controllable exciton localization and dynamics through spatially-modulated inter- and intralayer excitons in a MoSe 2 /WS 2 heterobilayer

Moiré heterobilayers exhibiting spatially varying exciton localization that can be precisely controlled through the twist angle have emerged as exciting platforms for studying complex quantum phenomena. Here, we study the exciton landscape in MoSe 2 /WS 2 heterobilayers through synergistic first-principles GW plus Bethe Salpeter equation (GW-BSE) calculations and complementary time- and angle-resolved photoemission spectroscopy (tr-ARPES). We find that the MoSe 2 /WS 2 heterobilayer has a type I band alignment at large twist angles. In contrast, at small twist angles, there exist simultaneous spatially modulated regions of local type I band alignment, hosting bright intralayer excitons, and local type II band alignment, hosting long-lived interlayer excitons, due to lattice reconstruction in different high-symmetry regions. In tr-ARPES this manifests in the observation of long-lived excitons with electron population in only MoSe 2 at large twist angles, while in samples with small twist angles, signals from two distinct long-lived exciton states with electron population in both layers are observed. Contrary to earlier studies, we find no excitonic hybridization near the low-energy absorption peaks in MoSe 2 /WS 2 , whose splitting can, instead, be explained by the lattice reconstruction.

Electronic properties and materials↗

DOE OSTI2021

Soil microbiome predictability increases with spatial and taxonomic scale

Soil microorganisms shape ecosystem function, yet it remains an open question whether we can predict the composition of the soil microbiome in places before observing it. Furthermore, it is unclear whether the predictability of microbial life exhibits taxonomic- and spatial-scale dependence, as it does for macrobiological communities. Here, we leverage multiple large-scale soil microbiome surveys to develop predictive models of bacterial and fungal community composition in soil, then test these models against independent soil microbial community surveys from across the continental United States. We find remark- able scale dependence in community predictability. The predictability of bacterial and fungal communities increases with the spatial scale of observation, and fungal predictability increases with taxonomic scale. These patterns suggest that there is an increasing importance of deterministic versus stochastic processes with scale, consistent with findings in plant and animal communities, suggesting a general scaling relationship across biology. Biogeochemical functional groups and high-level taxonomic groups of microorganisms were equally predictable, indicating that traits and taxonomy are both powerful lenses for understanding soil communities. Here, by focusing on out-of-sample prediction, these findings suggest an emerging generality in our understanding of the soil microbiome, and that this understanding is fundamentally scale dependent

Biogeography↗

DOE OSTI2024

Spatial variability in Arctic–boreal fire regimes influenced by environmental and human factors

Abstract Wildfire activity in Arctic and boreal regions is rapidly increasing, with severe consequences for climate and human health. Regional long-term variations in fire frequency and intensity characterize fire regimes. The spatial variability in Arctic–boreal fire regimes and their environmental and anthropogenic drivers, however, remain poorly understood. Here we present a fire tracking system to map the sub-daily evolution of all circumpolar Arctic–boreal fires between 2012 and 2023 using 375 m Visible Infrared Imaging Radiometer Suite active fire detections and the resulting dataset of the ignition time, location, size, duration, spread and intensity of individual fires. We use this dataset to classify the Arctic–boreal biomes into seven distinct ‘pyroregions’ with unique climatic and geographic environments. We find that these pyroregions exhibit varying responses to environmental drivers, with boreal North America, eastern Siberia and northern tundra regions showing the highest sensitivity to climate and lightning density. In addition, anthropogenic factors play an important role in influencing fire number and size, interacting with other factors. Understanding the spatial variability of fire regimes and its interconnected drivers in the Arctic–boreal domain is important for improving future predictions of fire activity and identifying areas at risk for extreme events.

Geology↗

DOE OSTI2019

Spatially dispersive circular photogalvanic effect in a Weyl semimetal

Weyl semimetals (WSMs) are gapless topological states of matter with broken inversion and/or time reversal symmetry. WSMs can support a circulating photocurrent when illuminated by circularly polarized light at normal incidence. Here, we report a spatially dispersive circular photogalvanic effect (s-CPGE) in a WSM that occurs with a spatially varying beam profile. Our analysis shows that the s-CPGE is controlled by a symmetry selection rule combined with asymmetric carrier excitation and relaxation dynamics. By evaluating the s-CPGE for a minimal model of a WSM, a frequency-dependent scaling behaviour of the photocurrent is obtained. Wavelength-dependent measurements from the visible to mid-infrared range show evidence of Berry curvature singularities and band inversion in the s-CPGE response. Here, we present the s-CPGE as a promising spectroscopic probe for topological band properties, with the potential for controlling photoresponse by patterning optical fields on topological materials to store, manipulate and transmit information.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Spatial complexity of carcass location influences vertebrate scavenger efficiency and species composition

Scavenging plays an important role in shaping communities through inter- and intra-specific interactions. Although vertebrate scavenger efficiency and species composition is likely influenced by the spatial complexity of environments, heterogeneity in carrion distribution has largely been disregarded in scavenging studies. We tested this hypothesis by experimentally placing juvenile bird carcasses on the ground and in nests in trees to simulate scenarios of nestling bird carrion availability. We used cameras to record scavengers removing carcasses and elapsed time to removal. Carrion placed on the ground was scavenged by a greater diversity of vertebrates and at > 2 times the rate of arboreal carcasses, suggesting arboreal carrion may represent an important resource to invertebrate scavengers, particularly in landscapes with efficient vertebrate scavenging communities. Nonetheless, six vertebrate species scavenged arboreal carcasses. Rat snakes (Elaphe obsolete), which exclusively scavenged from trees, and turkey vultures (Cathartes aura) were the primary scavengers of arboreal carrion, suggesting such resources are potentially an important pathway of nutrient acquisition for some volant and scansorial vertebrates. Our results highlight the intricacy of carrion-derived food web linkages, and how consideration of spatial complexity in carcass distribution (i.e., arboreal) may reveal important pathways of nutrient acquisition by invertebrate and vertebrate scavenging guilds.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2017

3D MALDI Mass Spectrometry Imaging of a Single Cell: Spatial Mapping of Lipids in the Embryonic Development of Zebrafish

The zebrafish ( Danio rerio ) has been widely used as a model vertebrate system to study lipid metabolism, the roles of lipids in diseases, and lipid dynamics in embryonic development. Here, we applied high-spatial resolution matrix-assisted laser desorption/ionization (MALDI)-mass spectrometry imaging (MSI) to map and visualize the three-dimensional spatial distribution of phospholipid classes, phosphatidylcholine (PC), phosphatidylethanolamines (PE), and phosphatidylinositol (PI), in newly fertilized individual zebrafish embryos. This is the first time MALDI-MSI has been applied for three dimensional chemical imaging of a single cell. PC molecular species are present inside the yolk in addition to the blastodisc, while PE and PI species are mostly absent in the yolk. Two-dimensional MSI was also studied for embryos at different cell stages (1-, 2-, 4-, 8-, and 16-cell stage) to investigate the localization changes of some lipids at various cell developmental stages. Lastly, four different normalization approaches were compared to find reliable relative quantification in 2D- and 3D- MALDI MSI data sets.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

Nanoscale Spatially Resolved Mapping of Uranium Enrichment

Abstract Spatially resolved analysis of uranium (U) isotopes in small volumes of actinide-bearing materials is critical for a variety of technical disciplines, including earth and planetary sciences, environmental monitoring, bioremediation, and the nuclear fuel cycle. However, achieving subnanometer-scale spatial resolution for such isotopic analysis is currently a challenge. By using atom probe tomography—a three-dimensional nanoscale characterisation technique—we demonstrate unprecedented nanoscale mapping of U isotopic enrichment with high sensitivity across various microstructural interfaces within small volumes (~100 nm 3 ) of depleted and low-enriched U alloyed with 10 wt% molybdenum that has different nominal enrichments of 0.20 and 19.75% 235 U, respectively. We map enrichment in various morphologies of a U carbide phase, the adjacent γ-UMo matrix, and across interfaces (e.g., carbide/matrix, grain boundary). Results indicate the U carbides were formed during casting, rather than retained from either highly enriched or depleted U feedstock materials. The approach presented here can be applied to study nanoscale variations of isotopic abundances in the broad class of actinide-bearing materials, providing unique insights into their origins and thermomechanical processing routes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Using active matter to introduce spatial heterogeneity to the susceptible infected recovered model of epidemic spreading

Abstract The widely used susceptible-infected-recovered (S-I-R) epidemic model assumes a uniform, well-mixed population, and incorporation of spatial heterogeneities remains a major challenge. Understanding failures of the mixing assumption is important for designing effective disease mitigation approaches. We combine a run-and-tumble self-propelled active matter system with an S-I-R model to capture the effects of spatial disorder. Working in the motility-induced phase separation regime both with and without quenched disorder, we find two epidemic regimes. For low transmissibility, quenched disorder lowers the frequency of epidemics and increases their average duration. For high transmissibility, the epidemic spreads as a front and the epidemic curves are less sensitive to quenched disorder; however, within this regime it is possible for quenched disorder to enhance the contagion by creating regions of higher particle densities. We discuss how this system could be realized using artificial swimmers with mobile optical traps operated on a feedback loop.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2024

Spatial control of perilacunar canalicular remodeling during lactation

Abstract Osteocytes locally remodel their surrounding tissue through perilacunar canalicular remodeling (PLR). During lactation, osteocytes remove minerals to satisfy the metabolic demand, resulting in increased lacunar volume, quantifiable with synchrotron X-ray radiation micro-tomography (SRµCT). Although the effects of lactation on PLR are well-studied, it remains unclear whether PLR occurs uniformly throughout the bone and what mechanisms prevent PLR from undermining bone quality. We used SRµCT imaging to conduct an in-depth spatial analysis of the impact of lactation and osteocyte-intrinsic MMP13 deletion on PLR in murine bone. We found larger lacunae undergoing PLR are located near canals in the mid-cortex or endosteum. We show lactation-induced hypomineralization occurs 14 µm away from lacunar edges, past a hypermineralized barrier. Our findings reveal that osteocyte-intrinsic MMP13 is crucial for lactation-induced PLR near lacunae in the mid-cortex but not for whole-bone resorption. This research highlights the spatial control of PLR on mineral distribution during lactation.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Spatial controls of methane uptake in upland soils across climatic and geological regions in Greenland

Abstract In the Arctic, the spatiotemporal variation of net methane uptake in upland soils depends on unresolved interactive controls between edaphic and microbial factors not yet included in current models, underpinning the uncertainty of upscaling the Arctic methane budget. Here we show that upland soils in Greenland are consistent methane sinks (−1.83 ± 0.19 nmol methane g −1 dw d −1 ) across a N-S (64–83 °N) pedoclimatic transect. We demonstrate that methane oxidizers abundance, soil pH, and available soil copper are important controls on the spatial variation in methane oxidation. We revised a soil biogeochemical model with a high-resolution land classification and meteorological data for Greenland and tested it against our methane uptake measurements. The model simulated well the magnitudes of observed methane uptake but not the spatial variation across all sites. This work provides novel insights into the controls of methane uptake, which are critical for the accuracy of methane budgets.

Environmental Sciences & Ecology↗

DOE OSTI2024

Spatial modeling algorithms for reactions and transport in biological cells

Biological cells rely on precise spatiotemporal coordination of biochemical reactions to control their functions. Such cell signaling networks have been a common focus for mathematical models, but they remain challenging to simulate, particularly in realistic cell geometries. Here we present Spatial Modeling Algorithms for Reactions and Transport (SMART), a software package that takes in high-level user specifications about cell signaling networks and then assembles and solves the associated mathematical systems. SMART uses state-of-the-art finite element analysis, via the FEniCS Project software, to efficiently and accurately resolve cell signaling events over discretized cellular and subcellular geometries. We demonstrate its application to several different biological systems, including yes-associated protein (YAP)/PDZ-binding motif (TAZ) mechanotransduction, calcium signaling in neurons and cardiomyocytes, and ATP generation in mitochondria. Throughout, we utilize experimentally derived realistic cellular geometries represented by well-conditioned tetrahedral meshes. These scenarios demonstrate the applicability, flexibility, accuracy and efficiency of SMART across a range of temporal and spatial scales.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2014

Spatially-resolved mapping of history-dependent coupled electrochemical and electronical behaviors of electroresistive NiO

Bias-induced oxygen ion dynamics underpins a broad spectrum of electroresistive and memristive phenomena in oxide materials. Although widely studied by device-level and local voltage-current spectroscopies, the relationship between electroresistive phenomena, local electrochemical behaviors, and microstructures remains elusive. Here, the interplay between history-dependent electronic transport and electrochemical phenomena in a NiO single crystalline thin film with a number of well-defined defect types is explored on the nanometer scale using an atomic force microscopy-based technique. A variety of electrochemically-active regions were observed and spatially resolved relationship between the electronic and electrochemical phenomena was revealed. The regions with pronounced electroresistive activity were further correlated with defects identified by scanning transmission electron microscopy. Using fully coupled mechanical-electrochemical modeling, we illustrate that the spatial distribution of strain plays an important role in electrochemical and electroresistive phenomena. In conclusion, these studies illustrate an approach for simultaneous mapping of the electronic and ionic transport on a single defective structure level such as dislocations or interfaces, and pave the way for creating libraries of defect-specific electrochemical responses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2017

Superior spatial resolution in confocal X-ray techniques using collimating channel array optics: elemental mapping and speciation in archaeological human bone

Confocal X-ray fluorescence imaging (CXFI) and confocal X-ray absorption spectroscopy (CXAS) respectively enable the study of three dimensionally resolved localization and speciation of elements. Applied to a thick sample, essentially any volume element of interest within the X-ray fluorescence escape depth can be examined without the need for physical thin sectioning. To date, X-ray confocal detection generally has employed a polycapillary optic in front of the detector to collect fluorescence from the probe volume formed at the intersection of its focus with the incident microfocus beam. This work demonstrates the capability of a novel Collimating Channel Array (CCA) optic in providing an improved and essentially energy independent depth resolution approaching 2 μm. By presenting a comparison of elemental maps of archaeological bone collected without confocal detection, and with polycapillary- and CCA-based confocal detection, this study highlights the strengths and limitations of each mode. Unlike the polycapillary, the CCA shows similar spatial resolution in maps for both low (Ca) and high (Pb and Sr) energy X-ray fluorescence, thus illustrating the energy independent nature of the CCA optic resolution. While superior spatial resolution is demonstrated for all of these elements, the most significant improvement is observed for Ca, demonstrating the advantage of employing the CCA optic in examining light elements. In addition to CXFI, this configuration also enables the collection of Pb L3 CXAS data from micro-volumes with dimensions comparable to bone microstructures of interest. Our CXAS result, which represents the first CCA-based biological CXAS, demonstrates the ability of CCA optics to collect site specific spectroscopic information. The demonstrated combination of site-specific elemental localization and speciation data will be useful in diverse fields.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2017

Improved spatial resolution for spot sampling in thermal desorption atomic force microscopy – mass spectrometry via rapid heating functions

The key to advancing materials is to understand and control their structure and chemistry. However, thorough chemical characterization is challenging since existing techniques characterize only a few properties of the specimen, thereby necessitating multiple measurement platforms to acquire the necessary information. The multimodal combination of atomic force microscopy (AFM) and mass spectrometry (MS) transcends existing analytical capabilities for nanometer scale spatially resolved correlation of the chemical and physical properties of a sample surface. One such hybrid system employs heated AFM cantilevers for thermal desorption (TD) sampling of molecules from a surface and subsequent gas phase ionization and detection of the liberated species by MS. Here in this paper, we report on the use of voltage pulse trains to tailor cantilever heating such that spot sampling size was reduced and mass spectral signal was improved compared to constant voltage, static heating of the cantilever. Desorption efficiency (DE), defined as the quotient of the mass spectral signal intensity and the volume of the desorption crater, was used to judge the effectiveness of a particular tailored heating function. To guide the development and optimization of the heating functions and aid in interpreting experimental results, a 1D finite element model was developed that predicted the cantilever response to different heating functions. Three tailored heating functions that used different combinations, magnitudes, and durations of rectangular voltage pulses, were used for surface spot sampling. The resultant sampling spot size and DE were compared to the same metrics obtained with the conventional method that uses a single voltage pulse. Using a model system composed of a thin film of ink containing pigment yellow 74 as a model system, desorption craters shrunk from 2 μm, using the conventional approach, to 310 nm using the optimum tailored heating function. This same pulsed heating function produced a 381× improvement in the DE and an 8× improvement in spatial resolution compared to the conventional heating approach showing that signal/amount of material sampled was improved significantly by this new cantilever heating strategy.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Spiers Memorial Lecture : Surface-enhanced Raman spectroscopy: from single particle/molecule spectroscopy to ångstrom-scale spatial resolution and femtosecond time resolution

Four decades on, surface-enhanced Raman spectroscopy (SERS) continues to be a vibrant field of research that is growing (approximately) exponentially in scope and applicability while pushing at the ultimate limits of sensitivity, spatial resolution, and time resolution. This introductory paper discusses some aspects related to all four of the themes for this Faraday Discussion. First, the wavelength-scanned SERS excitation spectroscopy (WS-SERES) of single nanosphere oligomers ( viz. , dimers, trimers, etc. ), the distance dependence of SERS, the magnitude of the chemical enhancement mechanism, and the progress toward developing surface-enhanced femtosecond stimulated Raman spectroscopy (SE-FSRS) are discussed. Second, our efforts to develop a continuous, minimally invasive, in vivo glucose sensor based on SERS are highlighted. Third, some aspects of our recent work in single molecule SERS and the translation of that effort to ångstrom-scale spatial resolution in ultrahigh vacuum tip-enhanced Raman spectroscopy (UHV-TERS) and single molecule electrochemistry using electrochemical (EC)-TERS will be presented. Finally, we provide an overview of analytical SERS with our viewpoints on SERS substrates, approaches to address the analyte generality problem ( i.e. target molecules that do not spontaneously adsorb and/or have Raman cross sections <10 -29 cm 2 sr -1 ), SERS for catalysis, and deep UV-SERS.

Chemistry↗

DOE OSTI2017

Spatial exciton allocation strategy with reduced energy loss for high-efficiency fluorescent/phosphorescent hybrid white organic light-emitting diodes

Due to the poor operational lifetime of blue phosphorescent dopants and blue thermally activated delayed fluorescent (TADF) materials, hybrid white organic light-emitting diodes (WOLEDs) with conventional blue fluorescent emitters are still preferred for commercial applications in general lighting. However, the improvement in the overall efficiency of hybrid WOLEDs has been limited due to energy losses during the energy transfer process and exciton quenching after the spatial separation of the singlet and triplet excitons. Here we demonstrate the development of a Spatial Exciton Allocation Strategy (SEAS) to achieve close to 100% internal quantum efficiency (IQE) in blue-yellow complementary color hybrid WOLEDs. The employed blue fluorophore not only has a resonant triplet level with the yellow phosphor to reduce energy loss during energy transfer processes and triplet–triplet annihilation (TTA), but also has a resonant singlet level with the electron transport layer to extend singlet exciton distribution and enhance both singlet and triplet exciton utilization. Thus, the resulting hybrid WOLEDs exhibited 104 lm W -1 efficacy at 100 cd m -2 and 74 lm W -1 at 1000 cd m -2 with CIE coordinates of (0.42, 0.44) which is warm white and suitable for indoor lighting.

36 MATERIALS SCIENCE↗

DOE OSTI2020

In situ X-ray spatial profiling reveals uneven compression of electrode assemblies and steep lateral gradients in lithium-ion coin cells

Coin cells are used extensively as test devices in battery research for evaluation of new materials and optimization of cycling protocols. Here, in situ X-ray diffraction profilometry is used to characterize spatial distribution of the active materials, lithiation, and phase distribution in electrodes of NCM523/graphite coin cells. The X-ray data indicate uneven areal compression of the electrode assembly in such cells, which we trace to a specific design feature that leads to elastic deformation of a metal spacer. Steep lithiation gradients observed in the electrodes imply radially-dependent resistivity, for which uneven compression of the separator is a likely cause. Electrochemical model calculations suggest that variable porosity of the polymer separator would account for the salient features of spatial profiles observed in these coin cells.

25 ENERGY STORAGE↗