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DOE OSTI2025

Diffusion Model-Guided Inverse Design of Bimetallic Catalysts for Ammonia Decomposition

In the past decade, artificial intelligence and deep learning have played increasingly prominent roles in materials design and discovery. Among these, generative AI models, known for their ability to create unique and complex structures, have emerged as state-of-the-art tools for materials screening due to their high efficiency and low computational cost. In catalysis, one of the major challenges is identifying promising material candidates within an immense chemical space. This challenge can be addressed using generative approaches, such as diffusion-based inverse design models. In this study, we present a machine learning-guided workflow that employed a diffusion model for the inverse design of bimetallic alloy catalysts for low-carbon ammonia decomposition, a key reaction for ammonia emission control and sustainable hydrogen production. Catalyst candidates were evaluated using nitrogen adsorption energy as the key descriptor, inspired by multiscale modeling. The proposed workflow identified low-cost, environmentally friendly catalysts with excellent catalytic performance, which have been validated theoretically and experimentally. Our framework decoupled the generative and property-prediction components, enhancing both flexibility and accuracy in the catalytic material design process.

Adsorption↗

DOE OSTI2025

Interfacial Cation Arrangement Controls Electrocatalytic Kinetics in CO 2 Reduction

The identity of electrolyte cations is known to strongly influence electrocatalytic activity, but the relationship between their interfacial arrangement and observed performance remains poorly understood. Organic cations, with their molecular tunability, provide a powerful platform for systematically probing these effects. Here, we leverage phosphonium-based geminal dications to control interfacial cation arrangement and identify the variables that most strongly influence catalytic rates. As a case study, we examine CO 2 reduction to CO over polycrystalline silver electrodes in dry aprotic acetonitrile. Through a combination of rotating disk electrode measurements, electrochemical impedance spectroscopy, and molecular dynamics simulations, we decouple the effects of cation–electrode distance and interfacial cation density on catalytic rates. We find that smaller, more densely packed cations induce stronger interfacial electric fields, which lower the activation barrier for CO 2 adsorption and increase reaction rates. Using geminal phosphonium dications [C n (P mmm ) 2 ][ClO 4 ] 2 , we demonstrate that both the vertical and lateral positioning of organic cations within the electrical double layer independently affect reactivity. These results demonstrate that electrolyte cation identity primarily influences catalytic kinetics by determining how efficiently charge can be arranged at electrochemical interfaces. Altogether, our findings support an electrostatic view of cation effects in catalysis and provide design principles for next-generation electrolytes.

Cations↗

DOE OSTI2026

Why Seeding Works When Nucleation Barriers Vanish

Crystallization is a process governed by the interplay between nucleation and growth. While crystalline seeds are known to reduce nucleation barriers and accelerate crystallization under nucleation-limited conditions, their influence when nucleation is not the limiting step remains poorly understood. This creates a mechanistic puzzle in systems where nucleation barriers are already negligible, yet seeding still accelerates crystallization. Here, the synthesis of zeolites is a quintessential example of growth-limited crystallization in which seeds accelerate the process despite negligible homogeneous nucleation barriers. Using coarse-grained molecular dynamics simulations─validated across two zeolites and the unrelated case of ice crystallization─we establish that growth-limited crystallization produces many small, misoriented crystallites whose slow coarsening into larger domains controls the emergence of X-ray-detectable crystallinity. Local crystalline order, structural coherence, and X-ray detectability are therefore kinetically decoupled milestones: the first can be reached rapidly while the latter two lag significantly. Seeds resolve this lag by imposing a common orientational registry on nascent crystallites, enabling their coherent coalescence into large seed-bound domains. This early coherence-building step produces a crystallite-size asymmetry that accelerates subsequent coarsening, advancing the onset of X-ray-detectable crystallinity without necessarily increasing the nucleated fraction. We conclude that under growth-limited conditions, the apparent induction period observed in powder X-ray diffraction reflects the time required to build long-range coherence, not the time to form crystalline material. Accordingly, seeds function not primarily by reducing nucleation barriers but by enforcing spatial coherence, thereby shortening the time required to develop long-range order detectable by X-ray diffraction.

Growth-Limited Crystallization↗

DOE OSTI2026

High-Rate, Selective Electrosynthesis of Cyclohexanone Oxime via In Situ Generation and Release of Hydroxylamine on Bismuth

Oxime compounds are key industrial intermediates for nylon precursors and commodity chemicals. However, conventional routes rely on multistep reactions and hydroxylamine (NH 2 OH) salts, raising significant safety and sustainability concerns. Although electrosynthesis offers an alternative, oxime formation on d-block transition metals suffers from poor selectivity, as nitrogen oxyanion intermediates bind strongly to the surface and are readily over-reduced to ammonia. Here, we report morphology-controlled p-block bismuth rhombic dodecahedra (Bi RDs) that promote in situ NH 2 OH generation and its desorption into the electrolyte, enabling an electrochemical-chemical decoupled route for cyclohexanone oxime (CHO) synthesis. Bi RDs deliver nearly 100% Faradaic efficiency (FE) at −0.5 V vs. RHE and a yield of 1.4 mmol h –1 cm –2 at −0.9 V vs. RHE in an H-cell, while maintaining a CHO selectivity of nearly 100% at 100 mA cm –2 in a flow cell. Under identical conditions, d-block electrodes (Cu, Pd, Ag) show FE below 30%. Density functional theory calculations reveal that Bi 6p orbital-derived surface states weaken intermediate binding and facilitate NH 2 OH desorption, suppressing over-reduction. Kinetic analysis, post-addition trapping experiments, and in situ ATR-FTIR and Raman spectroscopy suggest the following reaction mechanism: NH 2 OH is selectively generated at the electrode surface, released as a freely diffusing intermediate, and undergoes homogeneous condensation with cyclohexanone in the bulk electrolyte, bypassing the surface-confined Langmuir–Hinshelwood pathway. These findings demonstrate that regulating intermediate desorption through p-block orbital chemistry provides a general strategy for achieving high selectivity in electro-organic nitrogen synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Coupled Time-Lapse Full-Waveform Inversion for Subsurface Flow Problems Using Intrusive Automatic Differentiation

We describe a novel framework for estimating subsurface properties, such as rock permeability and porosity, from time-lapse observed seismic data by coupling full-waveform inversion (FWI), subsurface flow processes, and rock physics models. For the inverse modeling, we handle the back propagation of gradients by an intrusive automatic differentiation strategy that offers three levels of user control: (1) At the wave physics level, we adopted the discrete adjoint method in order to use our existing high-performance FWI code; (2) at the rock physics level, we used built-in automatic differentiation operators from the TensorFlow backend; (3) at the flow physics level, we implemented customized partial differential equation (PDE) operators for the multiphase flow equations. The three-level coupled inversion strategy strikes a good balance between computational efficiency and programming efforts, and when the gradients are chained together, it constitutes a coupled inverse system. Our numerical experiments demonstrate that the three-level coupled inverse problem is superior in terms of accuracy to a traditional decoupled inversion strategy. Additionally, our method is able to simultaneously invert for parameters in empirical relationships such as the rock physics models. Our proposed inverted model can be used for reservoir performance prediction and reservoir management/optimization purposes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Effects of Surface and Top Wind Shear on the Spatial Organization of Marine Stratocumulus-Topped Boundary Layers

Typically, the convective nature of Stratocumulus topped boundary layers (STBL) involves the motion of updrafts and downdrafts, driven by surface fluxes and radiative cooling, respectively. The balance between shear and buoyant forcings at the surface can determine the organization of updrafts between cellular and roll structures. We investigate the effect of varying shear at the surface and top of the STBL using Large Eddy Simulations, taking DYCOMS II RF01 as a base case. We focus on spatial identification of the following features: coherent updrafts and downdrafts, and observe how they are affected by varying shear. Stronger surface shear organizes the updrafts in rolls, causes less well-mixed thermodynamic profiles, and decreases cloud fraction and liquid water path (LWP). Stronger top shear also decreases cloud fraction and LWP more than surface shear, by thinning the cloud from the top. Features with stronger top than surface shear are associated with a net downward momentum transport and show early signs of decoupling. Classifying updrafts and downdrafts based on their vertical span and horizontal size confirms the dominance of tall objects spanning the whole STBL. Tall objects occupy 30% of the volume in the STBL, while short ones occupy less than 1%. For updraft and downdraft fluxes, these tall objects explain 65% of the vertical velocity variance and 83% of the buoyancy flux, on average. Stronger top shear also weakens the contribution of downdrafts to the turbulent fluxes and tilts the otherwise vertical development of updrafts.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Statistical Uncertainty in Paleoclimate Proxy Reconstructions

A quantitative analysis of any environment older than the instrumental record relies on proxies. Uncertainties associated with proxy reconstructions are often underestimated, which can lead to artificial conflict between different proxies, and between data and models. In this paper, using ordinary least squares linear regression as a common example, we describe a simple, robust and generalizable method for quantifying uncertainty in proxy reconstructions. We highlight the primary controls on the magnitude of uncertainty, and compare this simple estimate to equivalent estimates from Bayesian, nonparametric and fiducial statistical frameworks. We discuss when it may be possible to reduce uncertainties, and conclude that the unexplained variance in the calibration must always feature in the uncertainty in the reconstruction. This directs future research toward explaining as much of the variance in the calibration data as possible. We also advocate for a “data-forward” approach, that clearly decouples the presentation of proxy data from plausible environmental inferences.

58 GEOSCIENCES↗

DOE OSTI2021

Cloud Top Radiative Cooling Rate Drives Non-Precipitating Stratiform Cloud Responses to Aerosol Concentration

Increases in aerosol concentration are well known to influence the microphysical processes and radiative properties of clouds. By reducing droplet size, an increase in aerosol can lessen collision efficiency and increase liquid water path (LWP) in precipitating clouds or enhance evaporation rate and decrease LWP in non-precipitating clouds. We utilize large eddy simulations to further investigate these aerosol indirect effects in Arctic mixed-phase clouds and find, in agreement with previous studies, precipitating clouds to experience an increase in LWP and non-precipitating clouds a decrease in LWP. Most importantly however, our results reveal a different explanation for why such an LWP decrease occurs in decoupled, non-precipitating clouds. We find enhanced evaporation near cloud top to be driven primarily by a strengthening of maximum radiative cooling rate with aerosol concentration which drives stronger entrainment, an effect that holds true even in clouds that are optically thick.

58 GEOSCIENCES↗

DOE OSTI2021

Laboratory Verification of Electron-Scale Reconnection Regions Modulated by a Three-Dimensional Instability

We report that during magnetic reconnection in collisionless space plasma, the electron fluid decouples from the magnetic field within narrow current layers, and theoretical models for this process can be distinguished in terms of their predicted current layer widths. From theory, the off-diagonal stress in the electron pressure tensor is related to the thermal noncircular orbit motion of electrons around the magnetic field lines. This stress becomes significant when the width of the reconnecting current layer approaches the small characteristic length scale of the electron motion. To aid in situ spacecraft and numerical investigations of reconnection, the structure of the electron diffusion region is here investigated using the Terrestrial Reconnection Experiment. In agreement with the closely matched kinetic simulations, laboratory observations reveal the presence of electron-scale current layer widths. Although the layers are modulated by a current-driven instability, three-dimensional simulations demonstrate that it is the off-diagonal stress that is responsible for breaking the frozen-in condition of the electron fluid.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Distinct dynamical and structural properties of marine stratocumulus and shallow cumulus clouds in the Eastern North Atlantic

Low-level clouds in a marine environment are examined using multiple ground-based instruments. Here, we used Doppler radar and Doppler lidar measurements (1) to examine cloud properties including cloud base and top height and thickness and (2) to investigate vertical velocity (w) statistics throughout the subcloud and in-cloud layers. Marine stratocumulus (Sc) and shallow cumulus (Cu) clouds have distinct properties in their horizontal and vertical extent. We also find that the two cloud types have different thermodynamic (coupled and decoupled conditions) and dynamical characteristics for the first four moments of the w distributions (mean, variance, skewness, and kurtosis). We identify a strong dependence of subcloud mean w on near-surface horizontal wind direction, implying that topographic effects exert a substantial impact on boundary layer dynamics and cloud properties at Graciosa Island. Our findings strongly suggest that care must be taken when interpreting island-based observations as representative of a generic marine dynamical environment. This information also can be useful for guiding and constraining the future global model development using observational dataset.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Cloud Properties and Boundary Layer Stability Above Southern Ocean Sea Ice and Coastal Antarctica

Significant variability in climate predictions originates from the simulated cloud cover over the Southern Ocean. Historically, Southern Ocean cloud and aerosol properties have been less studied than their northern hemisphere counterparts, and cloud-sea-ice interactions over the Southern Ocean also remain largely unexamined. We used data from combined radar, lidar, radiometer, radiosonde, and ERA5 reanalysis profiles to investigate cloud property relationships to cloud temperature, sea-ice concentration, and boundary layer stability. Our findings show correlations between both cloud macrophysical properties and radiative effects and sea-ice concentration, and that the marine atmospheric boundary layer is more stable over higher sea-ice concentrations. Mixed-phase cloud frequency of occurrence was highest over the sea-ice zone at 15%, three times higher than over cold water south of the Antarctic Polar Front. For temperatures greater than –15°C, low-level, single-layer clouds were more likely to precipitate ice if they were coupled to cold-water or sea-ice surfaces than if they were decoupled from these surfaces, with the highest percentage of clouds precipitating ice observed over sea ice. These findings suggest a surface source of ice-nucleating particles at high southern latitudes that increases cloud glaciation probability. We discuss the implications of our results for future studies into the relationship between cloud properties, aerosols, sea ice, and boundary layer stability at high latitudes over the Southern Ocean.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Investigating the Diurnal Radiative, Turbulent, and Biophysical Processes in the Amazonian Canopy‐Atmosphere Interface by Combining LES Simulations and Observations

Abstract We investigate the atmospheric diurnal variability inside and above the Amazonian rainforest for a representative day during the dry season. To this end, we combine high‐resolution large‐eddy simulations that are constrained and evaluated against a comprehensive observation set, including CO 2 concentrations, gathered during GoAmazon2014/15. We design systematic numerical experiments to quantify whether a multilayer approach in solving the explicit canopy improves our canopy‐atmosphere representation. We particularly focus on the relationship between photosynthesis and plant transpiration, and their distribution at leaf and canopy scales. We found the variability of photosynthesis drivers like vapor pressure deficit and leaf temperature to be about 3 times larger for sunlit leaves compared to shaded leaves. This leads to a large spread on leaf stomatal conductance values with minimum and maximum values varying more than 100%. Regarding the turbulent structure, we find wind‐driven stripe‐like shapes at the canopy top and structures resembling convective cells at the canopy. Wind‐related variables provide the best spatiotemporal agreement between model and observations. The potential temperature and heat flux profiles agree with an observed decoupling near the canopy top interface, although with less variability and cold biases of up to 3 K. The increasing complexity on the biophysical processes leads to the largest disagreements for evaporation, CO 2 plant assimilation and soil efflux. The model is able to capture the correct dependences and trends with the magnitudes still differing. We finally discuss the need to revise leaf and soil models and to complete the observations at leaf and canopy levels.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Tonian Carbonates Record Phosphate-Rich Shallow Seas

The early-middle Neoproterozoic is thought to have witnessed significant perturbations to marine P cycling, in turn facilitating the rise of eukaryote-dominated primary production. However, with few robust constraints on aqueous P concentrations, current understanding of Neoproterozoic P cycling is generally model-dependent. To provide new geochemical constraints, we combined microanalytical data sets with solid-state Nuclear Magnetic Resonance, synchrotron-based X-ray Absorption Near Edge Structure spectroscopy, and micro-X-ray Fluorescence imaging to characterize the speciation and distribution of P in Tonian shallow-water carbonate rocks. These data reflect shallow water phosphate concentrations 10–100× higher than modern systems, supporting the hypothesis that tectonically-driven influxes in P periodically initiated kinetically-controlled CaCO 3 deposition, in turn destabilizing marine carbonate chemistry, climate, and nutrient inventories. Alongside these observations, a new compilation and statistical analysis of mudstone geochemistry data indicates that, in parallel, C org and P burial increased across later Tonian continental margins until becoming decoupled at the close of the Tonian, implicating widespread N-limitation triggered by increasing atmospheric O 2 .

58 GEOSCIENCES↗

DOE OSTI2023

Enhanced Cloud Top Longwave Radiative Cooling Due To the Effect of Horizontal Radiative Transfer in the Stratocumulus to Trade Cumulus Transition Regime

Abstract Recent studies develop the SPeedy Algorithm for Radiative TrAnsfer through CloUd Sides (SPARTACUS) to handle the influence of horizontal RT on vertical radiative fluxes within an atmospheric column. The present study applies SPARTACUS to large eddy simulation (LES)‐generated cloud fields across the stratocumulus to trade cumulus transition (STCT) regime with coarse and fine vertical resolutions. The results show that, as the vertical resolution increases, radiation simulations show increasingly stronger cloud‐top longwave (LW) radiative cooling. Consequently, the sharp radiative heating gradient across the cloud layer in the LES‐like resolution simulations cannot be resolved with the coarse resolution simulations. Including the horizontal RT typically enhances cloud LW radiative cooling rate by less than 10% for all the cloud fields but more significantly in the cloud fields during the STCT. The enhanced cloud LW radiative cooling also occurs in the lower cloud layer in the decoupled cumulus cloud regime.

Geology↗

DOE OSTI2023

The Role of Topography in Controlling Evapotranspiration Age

Abstract Evapotranspiration (ET) age is a key metric of water sustainability but a major unknown partly due to the extreme difficulty in modeling it. Groundwater is found to be important in ET age variations in small‐scale studies, yet our understanding is insufficient because groundwater systems are nested across scales. Here, we conducted GPU‐accelerated particle tracking with integrated hydrologic modeling to quantify the variations in ET age at a regional scale of ∼0.4 M km 2 . Simulation results reveal topography‐driven flow paths shaping the spatial and temporal patterns of ET age variations. On ridges, where root zone decoupling with deep subsurface storage, ET age is generally young, with seasonal variations dominated by meteorological conditions. In the valley bottom, ET age is generally old, with significant subseasonal variations caused by the convergence of subsurface flow paths. On hillslopes with water table depths ranging from 1 to 10 m, ET age shows strong seasonal variations caused by the connections with lateral groundwater regulated by ET demand. Our modeling approach provides insights into the basic linkages between ET age and topography at large scale. Our work highlights the perspective of multiscale studies of ET age, suggesting new field experiments to test these process connections and to determine if such linkages warrant inclusion in Earth System Models.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Formation of a Large Cold Groundwater Mantle Helium Anomaly and High Temperature Geothermal Resources in Response to Bimodal Magmatism Near Roosevelt Hot Springs and Utah FORGE, Milford Valley, Southwest Utah

Abstract A large mantle helium anomaly and separate domains of high heat flow are the predominant manifestations of bimodal magmatic activity in the Milford valley. The mantle helium anomaly (1.9–2.6 R/Ra) covers 270 km 2 and is subdivided into two separated domains: a cold shallow groundwater regime and high temperature hydrothermal activity. The zone of anomalous heat flow covers >100 km 2 and is also subdivided into two adjacent domains, comprising hydrothermal activity at Roosevelt Hot Springs (RHS) (3–7 W/m 2 ) and conductive heat flow (100–180 mW/m 2 ). While the transfer of heat and mantle helium at RHS are coupled, heat and helium transfer are decoupled in the adjacent cold groundwater regime to the west. Both the mantle helium and geothermal anomalies are attributed to recent mafic‐felsic magmatic intrusions of >400 km 3 , however, the absence of volcanic eruptions <500,000 years indicates magmas stall before rising to shallow crustal level <10 km depth. Deep level magmatism produces a felsic composition melt, which is inferred to be responsible for the widespread and near uniform range of diluted mantle helium values. A thick and impermeable mass of crystalline granitic basement rock at the mid‐crustal level divides the ascent of mantle helium into separate flow paths. It may also impede the rise of buoyant magma trapping thermal energy that facilitates partial melting, slow cooling, and development of a thick thermal aureole. Partitioning of convective and conductive thermal regimes and independent flow paths supplying deeply derived helium characterize the development of a large long‐lived magma‐related geothermal system.

Geochemistry & Geophysics↗

DOE OSTI2024

First Assessment of Cloud‐Land Coupling in LASSO Large‐Eddy Simulations

Abstract To enhance our understanding of cloud simulations over land, this study provides the first assessment of coupling between cloud and land surface in the Large‐Eddy Simulation (LES) Atmospheric Radiation Measurement Symbiotic Simulation and Observation (LASSO) activity for the shallow convection scenario. The analysis of observation data reveals a diurnal cycle of cloud‐land coupling, which co‐varies with surface fluxes. However, coupled (or decoupled) cumulus clouds are inadequately simulated, manifesting as a too‐high (or low) occurrence frequency during the afternoon. This discrepancy is mirrored by the overestimated cloud liquid water path and cloud‐top height. These overestimations are linked to the overpredicted boundary‐layer development and the easier trigger of shallow convection misrepresented in LES runs. Our study underscores the need to improve the representations of boundary‐layer processes and cloud‐land interactions within LES to better simulate shallow clouds in the future.

58 GEOSCIENCES↗

DOE OSTI2025

Factors Controlling Precipitation Onset and Maintenance: Inferences From Large Eddy Simulations of Two Afternoon Deep Convective Regimes Over Amazon

To investigate the environmental factors controlling the onset and maintenance of afternoon precipitation over tropical rainforests, two contrasting cases are created for large eddy simulations (LES) using GoAmazon observations: one features a single-pulse rain dissipating quickly in earlier afternoon, while the other shows double pulses lasting until evening. For these two specific cases under consideration, LES confirms that early-morning relative humidity dominates afternoon rain patterns. The attributed impacts are distinct: moisture determines the rain onset timing while temperature affects the peak rain intensity. Single-pulse day observes one round of strong precipitation and cold pools, which further suppresses convection. On double-pulse day, the first precipitation peak results from an intermediate development of congestus clouds, whose detrainment leads to a gradual moistening of the lower-to-middle troposphere. This behavior of convection favors a second pulse of stronger precipitation with more convective organization, whose development decouples from surface fluxes and sustains until evening.

Amazon↗