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Main Authors: Schwade, Martin, Zhang, Shaoming, Vonhoff, Frederik, Delgado, Frederico P., Egger, David A.
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2508.20536
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author Schwade, Martin
Zhang, Shaoming
Vonhoff, Frederik
Delgado, Frederico P.
Egger, David A.
author_facet Schwade, Martin
Zhang, Shaoming
Vonhoff, Frederik
Delgado, Frederico P.
Egger, David A.
contents Predicting optoelectronic properties of large-scale atomistic systems under realistic conditions is crucial for rational materials design, yet computationally prohibitive with first-principles simulations. Recent neural network models have shown promise in overcoming these challenges, but typically require large datasets and lack physical interpretability. Physics-inspired approximate models offer greater data efficiency and intuitive understanding, but often sacrifice accuracy and transferability. Here we present HAMSTER, a physics-informed machine learning framework for predicting the quantum-mechanical Hamiltonian of complex chemical systems. Starting from an approximate model encoding essential physical effects, HAMSTER captures the critical influence of dynamic environments on Hamiltonians using only few explicit first-principles calculations. We demonstrate our approach on halide perovskites, achieving accurate prediction of optoelectronic properties across temperature and compositional variations, and scalability to systems containing tens of thousands of atoms. This work highlights the power of physics-informed Hamiltonian learning for accurate and interpretable optoelectronic property prediction in large, complex systems.
format Preprint
id arxiv_https___arxiv_org_abs_2508_20536
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Physics-informed Hamiltonian learning for large-scale optoelectronic property prediction
Schwade, Martin
Zhang, Shaoming
Vonhoff, Frederik
Delgado, Frederico P.
Egger, David A.
Materials Science
Predicting optoelectronic properties of large-scale atomistic systems under realistic conditions is crucial for rational materials design, yet computationally prohibitive with first-principles simulations. Recent neural network models have shown promise in overcoming these challenges, but typically require large datasets and lack physical interpretability. Physics-inspired approximate models offer greater data efficiency and intuitive understanding, but often sacrifice accuracy and transferability. Here we present HAMSTER, a physics-informed machine learning framework for predicting the quantum-mechanical Hamiltonian of complex chemical systems. Starting from an approximate model encoding essential physical effects, HAMSTER captures the critical influence of dynamic environments on Hamiltonians using only few explicit first-principles calculations. We demonstrate our approach on halide perovskites, achieving accurate prediction of optoelectronic properties across temperature and compositional variations, and scalability to systems containing tens of thousands of atoms. This work highlights the power of physics-informed Hamiltonian learning for accurate and interpretable optoelectronic property prediction in large, complex systems.
title Physics-informed Hamiltonian learning for large-scale optoelectronic property prediction
topic Materials Science
url https://arxiv.org/abs/2508.20536