arXiv subjects

Detlef Hohl

Publications and source records attributed to Detlef Hohl.

14 recordsLinked to original sources

arXiv2026

Temperature-Induced Reorganization of Supported Zn$_3$ Clusters on Cu(111): From Minimum-Energy Structures to Finite-Temperature Ensembles

Understanding the nature of catalytic active sites under reaction conditions remains a central challenge in heterogeneous catalysis. In industrial copper/zinc oxide/alumina catalysts for methanol synthesis, small Zn-based species at the Cu interface have long been proposed as active-site candidates, yet their atomic-scale structure and stability remain controversial. Computational studies typically identify such species from optimized 0 K structures, assuming that minimum-energy configurations remain representative under reaction conditions. Here, we combine machine-learning-interatomic-potential-accelerated global optimization, molecular dynamics, and enhanced-sampling free-energy calculations to investigate supported Zn$_3$(OH)$_3$ and Zn$_3$(OH)$_2$CHOO clusters on Cu(111)-based surfaces from 0 to 450 K. While compact triangular configurations are generally favored among minimum-energy structures at 0 K, finite-temperature free-energy calculations reveal a pronounced shift toward extended linear configurations with increasing temperature. This transition is driven primarily by entropic stabilization and cannot be inferred from potential energies alone. Molecular dynamics further shows substantial cluster mobility on pristine Cu(111), indicating that long-term persistence depends not only on configurational stability but also on surface mobility. Surface Zn alloying strongly suppresses diffusion, thereby stabilizing isolated interfacial Zn species. Together, these results show that thermodynamically relevant structures of supported Zn-based clusters can differ fundamentally from static 0 K predictions because of competing enthalpic and entropic effects. Our findings highlight the limitations of identifying catalytic active sites solely from 0 K structures and underscore the importance of explicit finite-temperature sampling in catalyst modeling.

cond-mat.mtrl-sci↗

arXiv2026

Harnessing AtomisticSkills for Agentic Atomistic Research

Computational materials science and chemistry span vast knowledge domains and fractured software ecosystems. Although large language models (LLMs) have demonstrated research capabilities, scaling monolithic agents to manage the rigor and complexity of atomistic research remains a challenge. Here, we introduce AtomisticSkills, an open-source harness framework that empowers general-purpose AI coding agents to conduct atomistic research across materials science, chemistry, and drug discovery. By hierarchically decomposing scientific workflows into agent skills and tools, AtomisticSkills provides agents with modular, extensible, and plug-and-play research capabilities. The framework integrates more than 100 human-curated multidisciplinary skills, including database access, thermodynamics and kinetics modeling, and diverse simulation engines employing machine learning interatomic potentials (MLIPs) and density functional theory (DFT). We validate its functional coverage against scientific literature and demonstrate robust orchestration capabilities across diverse scientific campaigns: generative design of Li-ion solid-state electrolytes, high-throughput screening of metal-organic frameworks for CO2 capture, autonomous MLIP benchmarking and fine-tuning, multi-stage structure-based virtual screening for drug design, multimodal X-ray diffraction pattern analysis, and screening of Fe-oxide catalysts for oxygen evolution reaction. AtomisticSkills provides a critical agent infrastructure towards building fully autonomous AI scientists.

physics.chem-ph↗

arXiv2026

From Bulk to Surface: Structure and Dynamics of Amorphous Alumina from Deep Potential Molecular Dynamics

Understanding the atomic-scale structure and dynamics of amorphous oxide surfaces is essential for interpreting their chemical reactivity, mechanical stability, and interfacial behavior, yet direct experimental characterization remains challenging. We employ Deep Potential (DP) molecular dynamics to generate large-scale, ab initio-quality models of amorphous Al$_2$O$_3$ bulk glasses and melt-quenched free surfaces, enabling a quantitative analysis of both structure and relaxation dynamics with statistical confidence inaccessible to direct ab initio simulation. The trained DP model reproduces experimental liquid and glass structure, captures the cooling-rate dependence of the bulk glass transition, and corrects systematic biases in the polyhedral populations predicted by widely used classical force fields. At the free surface, mass density recovers to bulk values over ~10 $\unicode{x212B}$, while local coordination requires a slightly wider subsurface region to fully converge. The outermost layer is oxygen-enriched, exhibits altered polyhedral connectivity with contracted Al-O bonds, and hosts a broad population of under-coordinated motifs (notably AlO$_3$ and OAl$_2$) whose abundances are governed by glass stability. These reactive Lewis acid and Br$\unicode{x00F8}$nsted base sites are locally paired in a manner consistent with bond-valence compensation, yet remain spatially dispersed rather than aggregating into extended clusters. Despite this pronounced structural heterogeneity, the surface relaxes on the same timescale as the bulk and exhibits a comparable glass transition temperature, suggesting that the disordered surface is kinetically stable once formed. Together, these results establish a molecular-level picture of amorphous alumina surfaces and demonstrate the capability of machine-learned potentials to resolve structure-property relationships in disordered oxide interfaces.

cond-mat.mtrl-sci↗

arXiv2026

Partial recovery of meter-scale surface weather

Near-surface atmospheric conditions can differ sharply over tens to hundreds of meters due to land cover and topography, yet this variability is absent from current weather analyses and forecasts. It is unclear whether such meter-scale variability reflects irreducibly chaotic dynamics or contains a component predictable from surface characteristics and large-scale atmospheric forcing. Here we show that a substantial, physically coherent component of meter-scale near-surface weather is statistically recoverable from existing observations. By conditioning coarse atmospheric state on sparse surface station measurements and high-resolution Earth observation data, we infer spatially continuous fields of near-surface wind, temperature, and humidity at 10 m resolution across the contiguous United States. Relative to ERA5, the inferred fields reduce wind error by 29% and temperature and dewpoint error by 6%, while explaining substantially more spatial variance at fixed time steps. They also exhibit physically interpretable structure, including urban heat islands, evapotranspiration-driven humidity contrasts, and wind speed differences across land cover types. Our findings expand the frontier of weather modeling by demonstrating a computationally feasible approach to continental-scale meter-resolution inference. More broadly, they illustrate how conditioning coarse dynamical models on static fine-scale features can reveal previously unresolved components of the Earth system.

cs.LG↗

arXiv2025

Benchmarking Universal Machine Learning Interatomic Potentials for Supported Nanoparticles: Decoupling Energy Accuracy from Structural Exploration

Supported nanoparticle catalysts are widely used in the chemical industry. Computational modeling of supported nanoparticles based on density functional theory (DFT) often involves structural searches of stable local minimum energy configurations and molecular dynamics simulations at finite temperature. These are computationally demanding tasks that are intractable within DFT for large systems. In the last two decades, machine learning interatomic potentials (MLIPs) have been successfully used to substantially increase the size and time scales accessible to simulations approximating DFT accuracy. However, training reliable MLIPs is non-trivial as it requires many costly DFT calculations. Recently, several universal MLIPs (uMLIPs) have been developed, which are trained on large datasets that cover a wide range of molecules and materials. Here, we benchmark the accuracy and the efficiency of these uMLIPs in describing Cu nanoparticles supported on Al$_2$O$_3$ surfaces against our domain-specific DP-UniAlCu model. We find that the MACE-OMAT can reproduce reasonably well the low-energy structures found in global optimization at an energy accuracy comparable to DP-UniAlCu. Interestingly, the MatterSim-v1.0.0-1M model, which exhibits larger deviations in the binding energies, can find even more stable configurations than the other two models in some supported nanoparticle sizes, showing its capability in structure exploration. For MD simulations, MACE-OMAT and MatterSim-v1.0.0-1M can qualitatively reproduce the mean-squared displacements of Cu atoms (MSD$_\mathrm{Cu}$) predicted by DP-UniAlCu, albeit at roughly two orders of magnitude higher cost. We demonstrate that the uMLIPs can be very useful in simulating supported nanoparticles even without any fine-tuning, though their reduced efficiency remains a limiting factor for large-scale simulations.

cond-mat.mtrl-sci↗

arXiv2025

AI and the Net-Zero Journey: Energy Demand, Emissions, and the Potential for Transition

Thanks to the availability of massive amounts of data, computing resources, and advanced algorithms, AI has entered nearly every sector. This has sparked significant investment and interest, particularly in building data centers with the necessary hardware and software to develop and operate AI models and AI-based workflows. In this technical review article, we present energy consumption scenarios of data centers and impact on GHG emissions, considering both near-term projections (up to 2030) and long-term outlook (2035 and beyond). We address the quintessential question of whether AI will have a net positive, neutral, or negative impact on CO2 emissions by 2035. Additionally, we discuss AI's potential to automate, create efficient and disruptive workflows across various fields related to energy production, supply and consumption. In the near-term scenario, the growing demand for AI will likely strain computing resources, lead to increase in electricity consumption and therefore associated CO2 emissions. This is due to the power-hungry nature of big data centers and the requirements for training and running of large and complex AI models, as well as the penetration of AI assistant search and applications for public use. However, the long-term outlook could be more promising. AI has the potential to be a game-changer in CO2 reduction. Its ability to further automate and optimize processes across industries, from energy production to logistics, could significantly decrease our carbon footprint. This positive impact is anticipated to outweigh the initial emissions bump, creating value for businesses and society in areas where traditional solutions have fallen short. In essence, AI might cause some initial growing pains for the environment, but it has the potential to support climate mitigation efforts.

cs.AI↗

arXiv2025

Fourier Neural Operator based surrogates for $CO_2$ storage in realistic geologies

This study aims to develop surrogate models for accelerating decision making processes associated with carbon capture and storage (CCS) technologies. Selection of sub-surface $CO_2$ storage sites often necessitates expensive and involved simulations of $CO_2$ flow fields. Here, we develop a Fourier Neural Operator (FNO) based model for real-time, high-resolution simulation of $CO_2$ plume migration. The model is trained on a comprehensive dataset generated from realistic subsurface parameters and offers $O(10^5)$ computational acceleration with minimal sacrifice in prediction accuracy. We also explore super-resolution experiments to improve the computational cost of training the FNO based models. Additionally, we present various strategies for improving the reliability of predictions from the model, which is crucial while assessing actual geological sites. This novel framework, based on NVIDIA's Modulus library, will allow rapid screening of sites for CCS. The discussed workflows and strategies can be applied to other energy solutions like geothermal reservoir modeling and hydrogen storage. Our work scales scientific machine learning models to realistic 3D systems that are more consistent with real-life subsurface aquifers/reservoirs, paving the way for next-generation digital twins for subsurface CCS applications.

physics.comp-ph↗

arXiv2025

Dynamic Metal-Support Interaction Dictates Cu Nanoparticle Sintering on Al$_2$O$_3$ Surfaces

Nanoparticle sintering remains a critical challenge in heterogeneous catalysis. In this work, we present a unified deep potential (DP) model for Cu nanoparticles on three Al$_2$O$_3$ surfaces ($\gamma$-Al$_2$O$_3$(100), $\gamma$-Al$_2$O$_3$(110), and $\alpha$-Al$_2$O$_3$(0001)). Using DP-accelerated simulations, we reveal striking facet-dependent nanoparticle stability and mobility patterns across the three surfaces. The nanoparticles diffuse several times faster on $\alpha$-Al$_2$O$_3$(0001) than on $\gamma$-Al$_2$O$_3$(100) at 800 K while expected to be more sluggish based on their larger binding energy at 0 K. Diffusion is facilitated by dynamic metal-support interaction (MSI), where the Al atoms switch out of the surface plane to optimize contact with the nanoparticle and relax back to the plane as the nanoparticle moves away. In contrast, the MSI on $\gamma$-Al$_2$O$_3$(100) and on $\gamma$-Al$_2$O$_3$(110) is dominated by more stable and directional Cu-O bonds, consistent with the limited diffusion observed on these surfaces. Our extended long-time MD simulations provide quantitative insights into the sintering processes, showing that the dispersity of nanoparticles (the initial inter-nanoparticle distance) strongly influences coalescence driven by nanoparticle diffusion. We observed that the coalescence of Cu$_{13}$ nanoparticles on $\alpha$-Al$_2$O$_3$(0001) can occur in a short time (10 ns) at 800 K even with an initial inter-nanoparticle distance increased to 30 \r{A}, while the coalescence on $\gamma$-Al$_2$O$_3$(100) is inhibited significantly by increasing the initial inter-nanoparticle distance from 15 \r{A} to 30 \r{A}. These findings demonstrate that the dynamics of the supporting surface is crucial to understanding the sintering mechanism and offer guidance for designing sinter-resistant catalysts by engineering the support morphology.

cond-mat.mtrl-sci↗

arXiv2024

Local Off-Grid Weather Forecasting with Multi-Modal Earth Observation Data

Urgent applications like wildfire management and renewable energy generation require precise, localized weather forecasts near the Earth's surface. However, forecasts produced by machine learning models or numerical weather prediction systems are typically generated on large-scale regular grids, where direct downscaling fails to capture fine-grained, near-surface weather patterns. In this work, we propose a multi-modal transformer model trained end-to-end to downscale gridded forecasts to off-grid locations of interest. Our model directly combines local historical weather observations (e.g., wind, temperature, dewpoint) with gridded forecasts to produce locally accurate predictions at various lead times. Multiple data modalities are collected and concatenated at station-level locations, treated as a token at each station. Using self-attention, the token corresponding to the target location aggregates information from its neighboring tokens. Experiments using weather stations across the Northeastern United States show that our model outperforms a range of data-driven and non-data-driven off-grid forecasting methods. They also reveal that direct input of station data provides a phase shift in local weather forecasting accuracy, reducing the prediction error by up to 80% compared to pure gridded data based models. This approach demonstrates how to bridge the gap between large-scale weather models and locally accurate forecasts to support high-stakes, location-sensitive decision-making.

cs.LG↗

arXiv2020

Deep Neural Network Learning with Second-Order Optimizers -- a Practical Study with a Stochastic Quasi-Gauss-Newton Method

Training in supervised deep learning is computationally demanding, and the convergence behavior is usually not fully understood. We introduce and study a second-order stochastic quasi-Gauss-Newton (SQGN) optimization method that combines ideas from stochastic quasi-Newton methods, Gauss-Newton methods, and variance reduction to address this problem. SQGN provides excellent accuracy without the need for experimenting with many hyper-parameter configurations, which is often computationally prohibitive given the number of combinations and the cost of each training process. We discuss the implementation of SQGN with TensorFlow, and we compare its convergence and computational performance to selected first-order methods using the MNIST benchmark and a large-scale seismic tomography application from Earth science.

cs.LG↗

arXiv2018

Equation of state of fluid methane from first principles with machine learning potentials

The predictive simulation of molecular liquids requires models that are not only accurate, but computationally efficient enough to handle the large systems and long time scales required for reliable prediction of macroscopic properties. We present a new approach to the systematic approximation of the first-principles potential energy surface (PES) of molecular liquids using the GAP (Gaussian Approximation Potential) framework. The approach allows us to create potentials at several different levels of accuracy in reproducing the true PES, which allows us to test the level of quantum chemistry that is necessary to accurately predict its macroscopic properties. We test the approach by building potentials for liquid methane (CH$_4$), which is difficult to model from first principles because its behavior is dominated by weak dispersion interactions with a significant many-body component. We find that an accurate, consistent prediction of its bulk density across a wide range of temperature and pressure requires not only many-body dispersion, but also quantum nuclear effects to be modeled accurately.

physics.chem-ph↗

arXiv2017

A data-driven workflow for predicting horizontal well production using vertical well logs

In recent work, data-driven sweet spotting technique for shale plays previously explored with vertical wells has been proposed. Here, we extend this technique to multiple formations and formalize a general data-driven workflow to facilitate feature extraction from vertical well logs and predictive modeling of horizontal well production. We also develop an experimental framework that facilitates model selection and validation in a realistic drilling scenario. We present some experimental results using this methodology in a field with 90 vertical wells and 98 horizontal wells, showing that it can achieve better results in terms of predictive ability than kriging of known production values.

cs.OH↗

arXiv2016

Performance Analysis and Optimization of a Hybrid Distributed Reverse Time Migration Application

Applications to process seismic data employ scalable parallel systems to produce timely results. To fully exploit emerging processor architectures, application will need to employ threaded parallelism within a node and message passing across nodes. Today, MPI+OpenMP is the preferred programming model for this task. However, tuning hybrid programs for clusters is difficult. Performance tools can help users identify bottlenecks and uncover opportunities for improvement. This poster describes our experiences of applying Rice University's HPCToolkit and hardware performance counters to gain insight into an MPI+OpenMP code that performs Reverse Time Migration (RTM) on a cluster of multicore processors. The tools provided us with insights into the effectiveness of the domain decomposition strategy, the use of threaded parallelism, and functional unit utilization in individual cores. By applying insights obtained from the tools, we were able to improve the performance of the RTM code by roughly 30 percent.

cs.DC↗

arXiv2009

Theoretical investigation of methane under pressure

We present computer simulations of liquid and solid phases of condensed methane at pressures below 25 GPa, between 150 and 300 K, where no appreciable molecular dissociation occurs. We used molecular dynamics (MD) and metadynamics techniques, and empirical potentials in the rigid molecule approximation, whose validity was confirmed a posteriori by carrying out it ab initio MD simulations for selected pressure and temperature conditions. Our results for the melting line are in satisfactory agreement with existing measurements. We find that the fcc crystal transforms into a hcp structure with 4 molecules per unit cell (B phase) at about 10 GPa and 150 K, and that the B phase transforms into a monoclinic high pressure phase above 20 GPa. Our results for solid/solid phase transitions are consistent with those of Raman studies but the phase boundaries estimated in our calculations are at higher pressure than those inferred from spectroscopic data.

cond-mat.mtrl-sci↗