Interpolating many-body wave functions for accelerated molecular dynamics on the near-exact electronic surface
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arXiv
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| Auteurs principaux: | , |
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| Format: | Preprint |
| Publié: |
2024
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| _version_ | 1866916672234848256 |
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| author | Rath, Yannic Booth, George H. |
| author_facet | Rath, Yannic Booth, George H. |
| contents | While there have been many developments in computational probes of both strongly-correlated molecular systems and machine-learning accelerated molecular dynamics, there remains a significant gap in capabilities in simulating accurate non-local electronic structure over timescales on which atoms move. We develop an approach to bridge these fields with a practical interpolation scheme for the correlated many-electron state through the space of atomic configurations, whilst avoiding the exponential complexity of these underlying electronic states. With a small number of accurate correlated wave functions as a training set, we demonstrate provable convergence to near-exact potential energy surfaces for subsequent dynamics with propagation of a valid many-body wave function and inference of its variational energy whilst retaining a mean-field computational scaling. This represents a profoundly different paradigm to the direct interpolation of potential energy surfaces in established machine-learning approaches. We combine this with modern electronic structure approaches to systematically resolve molecular dynamics trajectories and converge thermodynamic quantities with a high-throughput of several million interpolated wave functions with explicit validation of their accuracy from only a few numerically exact quantum chemical calculations. We also highlight the comparison to traditional machine-learned potentials or dynamics on mean-field surfaces. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2402_11097 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Interpolating many-body wave functions for accelerated molecular dynamics on the near-exact electronic surface Rath, Yannic Booth, George H. Chemical Physics Strongly Correlated Electrons Computational Physics Quantum Physics While there have been many developments in computational probes of both strongly-correlated molecular systems and machine-learning accelerated molecular dynamics, there remains a significant gap in capabilities in simulating accurate non-local electronic structure over timescales on which atoms move. We develop an approach to bridge these fields with a practical interpolation scheme for the correlated many-electron state through the space of atomic configurations, whilst avoiding the exponential complexity of these underlying electronic states. With a small number of accurate correlated wave functions as a training set, we demonstrate provable convergence to near-exact potential energy surfaces for subsequent dynamics with propagation of a valid many-body wave function and inference of its variational energy whilst retaining a mean-field computational scaling. This represents a profoundly different paradigm to the direct interpolation of potential energy surfaces in established machine-learning approaches. We combine this with modern electronic structure approaches to systematically resolve molecular dynamics trajectories and converge thermodynamic quantities with a high-throughput of several million interpolated wave functions with explicit validation of their accuracy from only a few numerically exact quantum chemical calculations. We also highlight the comparison to traditional machine-learned potentials or dynamics on mean-field surfaces. |
| title | Interpolating many-body wave functions for accelerated molecular dynamics on the near-exact electronic surface |
| topic | Chemical Physics Strongly Correlated Electrons Computational Physics Quantum Physics |
| url | https://arxiv.org/abs/2402.11097 |