Results for “spatially explicit modeling” — Page 11

DOE OSTI2024

Estimates of Lake Nitrogen, Phosphorus, and Chlorophyll‐ a Concentrations to Characterize Harmful Algal Bloom Risk Across the United States

Abstract Excess nutrient pollution contributes to the formation of harmful algal blooms (HABs) that compromise fisheries and recreation and that can directly endanger human and animal health via cyanotoxins. Efforts to quantify the occurrence, drivers, and severity of HABs across large areas is difficult due to the resource intensive nature of field monitoring of lake nutrient and chlorophyll‐aconcentrations. To better characterize how nutrients interact with other environmental factors to produce algal blooms in freshwater systems, we used spatially explicit and temporally matched climate, landscape, in‐lake characteristic, and nutrient inventory data sets to predict nutrients and chlorophyll‐aacross the conterminous US (CONUS). Using a nested modeling approach, three random forest (RF) models were trained to explain the spatiotemporal variation in total nitrogen (TN), total phosphorus (TP), and chlorophyll‐aconcentrations across US EPA's National Lakes Assessment (n = 2,062). Concentrations of TN and TP were the most important predictors and, with other variables, the RF model accounted for 68% of variation in chlorophyll‐a. We then used these RF models to extrapolate lake TN and TP predictions to lakes without nutrient observations and predict chlorophyll‐afor ∼112,000 lakes across the CONUS. Risk for high chlorophyll‐aconcentrations is highest in the agriculturally dominated Midwest, but other areas of risk emerge in nutrient pollution hot spots across the country. These catchment and lake‐specific results can help managers identify potential nutrient pollution and chlorophyll‐ahot spots that may fuel blooms, prioritize at‐risk lakes for additional monitoring, and optimize management to protect human health and other environmental end goals.

Environmental Sciences & Ecology↗

DOE OSTI2020

High-resolution mapping of spatial heterogeneity in ice wedge polygon geomorphology near Prudhoe Bay, Alaska

It is well known that microtopography associated with ice wedge polygons drives pronounced, meter-scale spatial gradients in hydrologic and ecological processes on the tundra. However, highresolution maps of polygonal geomorphology are rarely available, due to the complexity and subtlety of ice wedge polygon relief at landscape scales. Here we present a sub-meter resolution map of >106 discrete ice wedge polygons across a ~1200 km2 landscape, delineated within a lidar-derived digital elevation model. The delineation procedure relies on a convolutional neural network paired with a set of common image processing operations and permits explicit measurement of relative elevation at the center of each ice wedge polygon. The resulting map visualizes meter- to kilometer-scale spatial gradients in polygonal geomorphology across an extensive landscape with unprecedented detail. This high-resolution inventory of polygonal geomorphology provides rich spatial context for extrapolating observations of environmental processes across the landscape. The map also represents an extensive baseline dataset for quantifying contemporary land surface deformation (i.e., thermokarst) at the survey area, through future topographic surveys.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2004

GMS-based"Future Time" Rainfall Data Assimilation for Mesoscale Weather Prediction over Korean Peninsula and Future Prospects with GPM Satellite Measurements

This study examines the use of satellite-derived nowcasted (short-term forecasted) rainfall over 3-hour time periods to gain an equivalent time increment in initializing a nonhydrostatic mesoscale model used for predicting convective rainfall events over the Korean peninsula. Infrared (IR) window measurements from the Japanese Geostationary Meteorological Satellite (GMS) are used to specify latent heating for a spinup period of the model - but in future time -- thus initializing in advance of actual time in the framework of a prediction scenario. The main scientific objective of the study is to investigate the strengths and weaknesses of this approach insofar as data assimilation, in which the nowcasted assimilation data are derived independently of the prognostic model itself. Although there have been various recent improvements in formulating the dynamics, thermodynamics, and microphysics of mesoscale models, as well as computer advances which allow the use of high resolution cloud-resolving grids and explicit latent heating over regional domains, spinup remains at the forefront of unresolved mesoscale modeling problems. In general, non-realistic spinup limits the skill in predicting the spatial-temporal distribution of convection and precipitation, primarily in the early hours of a. forecast, stemming from standard prognostic variables not representing the initial diabatic heating field produced by the ambient convection and cloud fields. The long-term goal of this research is to improve short-range (12-hour) quantitative precipitation forecasting (QPF) over the Korean peninsula through the use of innovative data assimilation methods based on geosynchronous satellite measurements. As a step in th~s direction, a non-standard data assimilation experiment in conjunction with GMS-retrieved nowcasted rainfall information introduced to the mesoscale model is conducted. The 3-hourly precipitation forecast information is assimilated through nudging the associated diabatic heating during the early stages of a forecast period. This procedure is expected to enhance details in the moisture field during model integration, and thus improve spinup performance, assuming the errors in the future time latent heating data ate less than intrinsic model background errors.

Smith, Eric A.↗

NASA NTRS1985

Radial diffusion in magnetodiscs

The orbits of charged particles in magnetodiscs are considered. The bounce motion is assumed adiabatic except for transits of a small equatorial region of weak magnetic field strength and high field curvature. Previous theory and modeling have shown that particles scatter randomly in pitch angle with each passage through the equator. A peaked distribution thus diffuses in pitch angle on the time scale of many bounces. It is argued in this paper that spatial diffusion is a further consequence when the magnetodisc has a longitudinal asymmetry. A general expression for DLL, the diffusion of equatorial crossing radii, is derived. DLL is evaluated explicitly for ions in Jupiter's 20-35 radii magnetodisc, assumed to be represented by Connerney et al.'s (1982) Voyager model plus a small image dipole asymmetry. Rates are energy, species, and space dependent but can average as much as a few tenths of a planetary radius per bounce period.

Birmingham, T. J.↗

DOE OSTI2020

Calculation of the detonation state of HN 3 with quantum accuracy

HN 3 is a unique liquid energetic material that exhibits ultrafast detonation chemistry and a transition to metallic states during detonation. We combine the Chebyshev interaction model for efficient simulation (ChIMES) many-body reactive force field and the extended-Lagrangian multiscale shock technique molecular dynamics method to calculate the detonation properties of HN 3 with the accuracy of Kohn–Sham density-functional theory. ChIMES is based on a Chebyshev polynomial expansion and can accurately reproduce density-functional theory molecular dynamics (DFT-MD) simulations for a wide range of unreactive and decomposition conditions of liquid HN 3 . We show that addition of random displacement configurations and the energies of gas-phase equilibrium products in the training set allows ChIMES to efficiently explore the complex potential energy surface. Schemes for selecting force field parameters and the inclusion of stress tensor and energy data in the training set are examined. Structural and dynamical properties and chemistry predictions for the resulting models are benchmarked against DFT-MD. We demonstrate that the inclusion of explicit four-body energy terms is necessary to capture the potential energy surface across a wide range of conditions. Our results generally retain the accuracy of DFT-MD while yielding a high degree of computational efficiency, allowing simulations to approach orders of magnitude larger time and spatial scales. The techniques and recipes for MD model creation we present allow for direct simulation of nanosecond shock compression experiments and calculation of the detonation properties of materials with the accuracy of Kohn–Sham density-functional theory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Characterization factors and other air quality impact metrics: Case study for PM 2.5 -emitting area sources from biofuel feedstock supply

In this paper, we develop a framework and metrics for estimating the impact of emission sources on regulatory compliance and human health for applications in air quality planning and life cycle impact assessment (LCIA). Our framework is based on a pollutant's characterization factor (CF) and three new metrics: Available Regulatory Capacity for Incremental Emissions (ARCIE), Source CF Ratio, and Activity Health Impact (AHI) Ratio. ARCIE can be used to assess whether a receptor location has capacity to accommodate additional source emissions while complying with regulatory limits. We present CF as a midpoint indicator of health impacts per unit mass of emitted pollutant. Source CF Ratio enables comparison of potential new-source locations based on human health impacts. The AHI Ratio estimates the health impacts of a pollutant in relation to the utilization of the source for each unit of product or service. These metrics can be applied to any pollutant, energy source sector (e.g., agriculture, electricity), source type (point, line, area), and spatial modeling domain (nation, state, city, region). We demonstrate these metrics through a case study of fine particulate (PM 2.5 ) emissions from U.S. corn stover harvesting and local processing at various scales, representing steps in the biofuel production process. We model PM 2.5 formation in the atmosphere using a novel reduced-complexity chemical transport model called the Intervention Model for Air Pollution (InMAP). Through this case study, we present the first area-source PM 2.5 CFs that address the recommendations of several LCIA studies to establish spatially explicit CFs specific to an energy source sector or type. Overall, the framework developed in this work provides multiple new ways to consider the potential impacts of air emissions through spatially differentiated metrics.

09 BIOMASS FUELS↗

DOE OSTI2020

Controlling protein adsorption modes electrostatically

Protein adsorption on surfaces is ubiquitous in biology and in biotechnology. There are various forces required for controlling protein adsorption. Here, we introduce an explicit ion coarse-grained molecular dynamics simulation approach for studying the effects of electrostatics on protein adsorption, and 2D protein assembly on charged surfaces. Our model accounts for the spatial distribution of protein charges. We use catalase as our model protein. We find that the preferential adsorption mode of proteins at low protein concentration on a charged surface is “standing up”. When the protein concentration in a solution increases to reach a critical density on the surface, the adsorption mode switches from “standing up” to a mixed state “flat on” and “standing up”, which increases the lateral correlations among the adsorbed proteins. As such, the changes in the adsorption mode arise from the protein adsorption that cancel the surface charge and the protein–protein repulsion. This correlated surface structure melts as the salt concentration increases because the charged surface is cancelled by the salt ions and the proteins de-adsorb. For the case of strongly charged surfaces the “standing up” conformation remains more favorable even at high protein adsorption at low salt concentrations since in that conformation the surface charge is cancelled more effectively, generating an even more laterally correlated structure. We elucidate the effects of parameters such as surface charge density, salt concentration, and protein charges on the different adsorption modes and the structure and organization of proteins on the charged surfaces. Finally, this study provides a guide for controlling protein assembly on surfaces.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

Bosonization in three spatial dimensions and a 2-form gauge theory

We describe a 3d analog of the Jordan-Wigner transformation which maps an arbitrary fermionic system on a 3d spatial lattice to a 2-form Z 2 gauge theory with an unusual Gauss law. An important property of this map is that it preserves the locality of the Hamiltonian. Here, the map depends explicitly on the choice of a spin structure of the spatial manifold. We give examples of 3d bosonic systems dual to free fermions. We also describe the corresponding Euclidean lattice models, which is analogous to the Steenrod square term in (3+1)D [compared to the Chern-Simon term in (2+1)D].

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Southern Company Services: Project 2: Tall Tower Wind Technical Potential for the Southeast (Modifications 4, 5), Project 4: Offshore Wind Potential for Southern Company Services (Modifications 7, 8)

Project 2: The National Laboratory of the Rockies (NLR) and Southern Company Services (SCS) seek to establish an agreement to assess the technical potential for wind energy in the Southeastern U.S. SCS has requested that NLR conduct a detailed assessment of system performance, available capacity, transmission distance, and levelized cost of electricity (LCOE) at turbine hub heights of 100m to 160m within the SCS service territory. NLR will also provide an assessment of utility photovoltaic (PV) technical potential within the SCS service territory. NLR has unique modeling capabilities to assist SCS with high spatial and temporal resolution assessment of wind and PV technical potential, considering geospatial constraints. Project 4: NLR and SCS seek to develop a spatially explicit techno-economic assessment for offshore wind energy in the Southeastern U.S. The analysis aims to characterize the regional sensitivities of offshore wind plant costs and performance, underwater cabling, potential siting constraints, and landfall spur transmission costs.

17 WIND ENERGY↗

DOE OSTI2025

Supporting Information - How Can Crop Production Adapt to growing groundwater restrictions in the West?

Abstract This data plan outlines the structure and content of datasets generated and utilized in the research presented in the manuscript abstract. Groundwater overdraft has led to serious water supply issues in the US West. Most western states manage groundwater use through a permitting system, but California has only recently begun to restrict groundwater use statewide with the 2014 passage of groundwater restrictions which target the elimination of groundwater overdraft practices by 2042. With groundwater extraction curtailed, crop production in the US West (a $95 billion industry annually) will be affected, and appropriate response strategies will be needed to ensure minimal disruption to food production and the regional economy. In this paper, we explore the adoption of alternative adaptive responses: (a) deficit irrigation; (b) switching to less water-intensive crops; (c) changing the extent of irrigated land (including fallowing); and (d) geographically shifting crop production. Employing an integrated modeling approach, we explicitly capture the interactions and feedbacks between local hydrology, changes in crop yields, crop and land use decision-making, changes in crop prices, and regional shifts in crop production. We find that the optimal adaptive response is spatially heterogeneous and comprises a portfolio of strategies. Southwestern states and California will be the most impacted by groundwater restrictions. The optimal responses in these states are to both adopt deficit irrigation strategies and reduce a portion of their irrigated croplands, resulting in a shift in crop production to northwestern states with a larger supply of water. The datasets detailed in this repository represent the output from these integrated models, specifically designed to support the analysis and visualization presented in the manuscript and supplemental information. These datasets, used in conjunction with the scripts available at our associated GitHub repository (https://github.com/pches/Femeena_etal_How_can_crop_production_adapt), enable the reproduction of figures and facilitate a comprehensive understanding of the optimal adaptive strategies in agriculture for mitigating water stress under varying groundwater extraction scenarios, as outlined in the abstract.

DNDCe↗

DOE OSTI2025

Supporting Information - How Can Crop Production Adapt to growing groundwater restrictions in the West?

Abstract This data plan outlines the structure and content of datasets generated and utilized in the research presented in the manuscript abstract. Groundwater overdraft has led to serious water supply issues in the US West. Most western states manage groundwater use through a permitting system, but California has only recently begun to restrict groundwater use statewide with the 2014 passage of groundwater restrictions which target the elimination of groundwater overdraft practices by 2042. With groundwater extraction curtailed, crop production in the US West (a $95 billion industry annually) will be affected, and appropriate response strategies will be needed to ensure minimal disruption to food production and the regional economy. In this paper, we explore the adoption of alternative adaptive responses: (a) deficit irrigation; (b) switching to less water-intensive crops; (c) changing the extent of irrigated land (including fallowing); and (d) geographically shifting crop production. Employing an integrated modeling approach, we explicitly capture the interactions and feedbacks between local hydrology, changes in crop yields, crop and land use decision-making, changes in crop prices, and regional shifts in crop production. We find that the optimal adaptive response is spatially heterogeneous and comprises a portfolio of strategies. Southwestern states and California will be the most impacted by groundwater restrictions. The optimal responses in these states are to both adopt deficit irrigation strategies and reduce a portion of their irrigated croplands, resulting in a shift in crop production to northwestern states with a larger supply of water. The datasets detailed in this repository represent the output from these integrated models, specifically designed to support the analysis and visualization presented in the manuscript and supplemental information. These datasets, used in conjunction with the scripts available at our associated GitHub repository (https://github.com/pches/Femeena_etal_How_can_crop_production_adapt), enable the reproduction of figures and facilitate a comprehensive understanding of the optimal adaptive strategies in agriculture for mitigating water stress under varying groundwater extraction scenarios, as outlined in the abstract.

DNDCe↗

DOE OSTI2025

Supporting Information - How Can Crop Production Adapt to growing groundwater restrictions in the West?

Abstract This data plan outlines the structure and content of datasets generated and utilized in the research presented in the manuscript abstract. Groundwater overdraft has led to serious water supply issues in the US West. Most western states manage groundwater use through a permitting system, but California has only recently begun to restrict groundwater use statewide with the 2014 passage of groundwater restrictions which target the elimination of groundwater overdraft practices by 2042. With groundwater extraction curtailed, crop production in the US West (a $95 billion industry annually) will be affected, and appropriate response strategies will be needed to ensure minimal disruption to food production and the regional economy. In this paper, we explore the adoption of alternative adaptive responses: (a) deficit irrigation; (b) switching to less water-intensive crops; (c) changing the extent of irrigated land (including fallowing); and (d) geographically shifting crop production. Employing an integrated modeling approach, we explicitly capture the interactions and feedbacks between local hydrology, changes in crop yields, crop and land use decision-making, changes in crop prices, and regional shifts in crop production. We find that the optimal adaptive response is spatially heterogeneous and comprises a portfolio of strategies. Southwestern states and California will be the most impacted by groundwater restrictions. The optimal responses in these states are to both adopt deficit irrigation strategies and reduce a portion of their irrigated croplands, resulting in a shift in crop production to northwestern states with a larger supply of water. The datasets detailed in this repository represent the output from these integrated models, specifically designed to support the analysis and visualization presented in the manuscript and supplemental information. These datasets, used in conjunction with the scripts available at our associated GitHub repository (https://github.com/pches/Femeena_etal_How_can_crop_production_adapt), enable the reproduction of figures and facilitate a comprehensive understanding of the optimal adaptive strategies in agriculture for mitigating water stress under varying groundwater extraction scenarios, as outlined in the abstract.

DNDCe↗

DOE OSTI2026

Data for A Hybrid Biophysical-Machine Learning Framework for Diurnal Surface Energy Flux Estimation Using Proximal Sensing

Thermal infrared-based remote sensing of surface energy fluxes has traditionally relied on high spatial resolution satellite data with revisit frequencies on the order of weeks. In this study, we evaluate a biophysics-based analytical surface energy balance model for predicting latent energy (LE) and sensible heat (H) fluxes using proximal sensing observations. The Surface Temperature Initiated Closure (STIC1.2) model has been extensively validated across a wide range of spatial and temporal scales using various satellite-derived thermal infrared data sets. Here we extend this validation by applying STIC at sub-hourly temporal resolution over multiple growing seasons for four distinct agricultural systems. We further develop and evaluate novel STIC variants that incorporate machine learning (ML) techniques to eliminate the need for surface energy balance observations, specifically net radiation and soil heat flux, thereby enhancing model applicability in data-sparse settings. The integration of a ML component to estimate surface available energy is shown to have strong predictive performance for both LE (R2 = 0.81–0.94) and H (R2 = 0.46–0.72) across all agricultural systems examined here, demonstrating the potential of hybrid biophysical-machine learning approaches for surface energy balance modeling with minimal data requirements. This study concludes with a novel application of explainable machine learning (exML) to diagnose sources of model error. This exML framework attributes residual prediction errors to both model input variables and environmental drivers not explicitly included in the simulation experiments. This approach provides a new pathway for improving model design and integrating previously overlooked yet influential variables into future model iterations.

AI/ML↗

NASA NTRS2003

Jet Noise Physics and Modeling Using First-principles Simulations

An extensive analysis of our jet DNS database has provided for the first time the complex correlations that are the core of many statistical jet noise models, including MGBK. We have also for the first time explicitly computed the noise from different components of a commonly used noise source as proposed in many modeling approaches. Key findings are: (1) While two-point (space and time) velocity statistics are well-fitted by decaying exponentials, even for our low-Reynolds-number jet, spatially integrated fourth-order space/retarded-time correlations, which constitute the noise "source" in MGBK, are instead well-fitted by Gaussians. The width of these Gaussians depends (by a factor of 2) on which components are considered. This is counter to current modeling practice, (2) A standard decomposition of the Lighthill source is shown by direct evaluation to be somewhat artificial since the noise from these nominally separate components is in fact highly correlated. We anticipate that the same will be the case for the Lilley source, and (3) The far-field sound is computed in a way that explicitly includes all quadrupole cancellations, yet evaluating the Lighthill integral for only a small part of the jet yields a far-field noise far louder than that from the whole jet due to missing nonquadrupole cancellations. Details of this study are discussed in a draft of a paper included as appendix A.

Freund, Jonathan B.↗

DOE OSTI2020

A buoyancy–shear–drag-based turbulence model for Rayleigh–Taylor, reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz mixing

A phenomenological turbulence model for Rayleigh–Taylor, reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz instability-induced mixing is developed using a general buoyancy–shear–drag model. Analytic solutions to the simplified model equations corresponding to each instability are derived separately, which are then used to calibrate the model coefficients to predict specific values of the mixing layer growth parameters and exponents. The buoyancy-shear–drag equations for the bubble and spike mixing layer widths are then solved numerically, and a turbulent diffusivity (or viscosity) is constructed dimensionally as the product of the mixing layer width, h, and its time-derivative, dh/dt. Surrogate turbulent fields are then constructed by multiplying a presumed, approximate self-similar spatial profile by appropriate functions of h and dh/dt. Using several simplifying approximations, the turbulent diffusion equations satisfied by the mean mass fraction and mean shear velocity are solved analytically in a reference frame moving with the mean advection velocity, and it is shown that the mean fields evolve in space and time as expected. The explicit modeling and solution of turbulent transport equations (e.g., for the turbulent kinetic energy and its dissipation rate or a lengthscale) are not required. By using separate equations for the bubble and spike evolution, the model naturally captures the asymmetry induced by an increasing density contrast between the heavy and light fluids. The model also includes molecular dissipation and diffusion, and therefore, can describe transition to fully-developed turbulence if the initial turbulent diffusivity/viscosity is much smaller than the molecular diffusivity/viscosity. This model is applied to constant-acceleration Rayleigh–Taylor, impulsively reshocked Richtmyer–Meshkov, and variable-density Kelvin–Helmholtz mixing layers to demonstrate its utility. It is shown that the numerical solutions of the model calibrated using specific values of the instability growth parameters and exponents: (1) produces mixing layer widths in agreement with the expected self-similar growth power laws; (2) gives spatiotemporal profiles of turbulent fields that are expected and consistent with previous results; (3) predicts the expected power-law growths and decays of the spatially-integrated turbulent fields, and; (4) gives spatiotemporal profiles of the mean fields that are expected and consistent with previous results. This relatively simple model can be implemented numerically, and is expected to be useful for fundamental as well as astrophysical and inertial confinement fusion applications.

42 ENGINEERING↗

NASA NTRS1993

Grand challenge scientific questions in coupled modeling

Most convective field experiments in the past (e.g., SESAME, CCOPE, CINDE) have attempted to resolve only the immediate scales of moist convection using network arrays that spanned two or three atmospheric scales at most. Furthermore, these scales have been defined more on practical considerations (cost, manpower, etc.) than on a clear understanding of their theoretical significance. Unfortunately, this has precluded a description of the entire life cycle of MCS's and their interaction with larger scale systems, the land surface, and trace species. Fortunately, the following factors now make it possible to attempt to simulate scale contraction processes from the synoptic scale down to the cloud scale, as well as interactions between complex meteorological, land surface, precipitation, chemical, and hydrologic processes with coupled, multiscale models: the availability of new technology to sample meteorological fields at high temporal and spatial resolution over a broad region made possible by the weather observing modernization program; increased computer power and improved numerical approaches to run limited area models with nonhydrostatic precipitation physics so as to explicitly resolve MCS (Mesoscale Convective System) processes; and four dimensional assimilation of non-conventional data to provide dynamically consistent datasets for diagnostic analysis of nonlinear scale-interactive dynamics. Several examples of scale-interactive processes which present grand challenges for coupled, multiscale modeling were presented.

Koch, Steven↗

DOE OSTI2022

Representing Global Soil Erosion and Sediment Flux in Earth System Models

Abstract Soil erosion produces enormous amounts of sediment, carbon, and nutrient fluxes from land to rivers, thus playing crucial roles in global biogeochemical cycles and food security. To predict soil erosion in the context of climate and land use changes, we explicitly parameterize cropland management actions (i.e., irrigation, conserved agriculture, and crop residue management) and geological factors (i.e., lithology and glacier) in the Energy Exascale Earth System Model (E3SM) soil erosion module. The erosion model is calibrated using a global‐scale regionalized parameter calibration method. The spatial variabilities of the modeled and the Revised Universal Soil Loss Equation (RUSLE) based benchmark soil erosion are consistent across vegetation, climate and soil properties. Compared with independent data, our model shows a bias reduction in 59% of the observations relative to the RUSLE‐based soil erosion, with 53% of the bias reduction exceeding 50%. This improvement is mainly due to a better representation of the topographic effect on soil erosion. Our results indicate that conserved agriculture practices have effectively reduced soil erosion in cropland by over 25% in the United States and Argentina. In contrast, irrigation has increased soil erosion in many Asian countries. For upland sediment flux, our model is consistent with the WBMsed benchmark data in inter‐basin variability but could be more skillful in simulating intra‐basin variability because it couples soil erosion and sediment flux explicitly. The developed model provides useful skills for more realistic predictions of soil erosion and river sediment dynamics under environmental changes.

58 GEOSCIENCES↗

DOE OSTI2024

Structural regulation-induced Li-electron disentanglement for stabilized oxygen redox of Li-excess disordered rock-salt cathode materials

Since the discovery of its electrochemical activity, Li-excess disordered rock-salt (DRX) cathode material has received worldwide attention as it sets up a new way to exploit oxygen redox beyond the conventional layered structure with late-3d transition metals. However, the intricate structure-function relationship in the disordered lattice of the DRX material fogs the researcher's lens on the underlying redox mechanisms. Here, in this study, we employ a synergistic approach combining neutron total scattering with reverse Monte Carlo modeling and density functional theory calculations to unravel the landscape of oxygen redox reactions in DRX. Redox activities are evaluated in diverse oxygen clusters (OLi x TM 6-x ) and the spatial distribution of these clusters in the model DRX structure (Li 1.16 Ti 0.37 Ni 0.37 Nb 0.1 O 2 and Li 1.2 Ti 0.35 Ni 0.35 Nb 0.1 O 1.8 F 0.2 ) is explicitly determined. The results unveil that by regulating the short-range ordering between cations, fluorine atoms can effectively decouple the location of Li extraction and electron depletion. Such disentanglement between the Li reservoir and electron reservoir in the DRX lattice could play a pivotal role in protecting the oxidized oxygen and preserving the lattice framework during cycling. Through a tentatively designed non-fluorinated DRX oxide realizing similar Li-electron decoupling, an obvious enhancement of the cycling capability can be achieved without compromising the capacity release.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗