Preprint

PUBDB-2023-05097

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Computing excited states of molecules using normalizing flows

Saleh, Y. (Corresponding author)CFEL*DESY* ; Fernandez Corral, A.CFEL*DESY* ; Iske, A.CFEL*Extern* ; Küpper, J.CFEL*XFEL.EU*DESY* ; Yachmenev, A.CFEL*DESY*

2023

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Report No.: arXiv:2308.16468

Abstract: We present a new nonlinear variational framework for simultaneously computing ground and excited states of quantum systems. Our approach is based on approximating wavefunctions in the linear span of basis functions that are augmented and optimized \emph{via} composition with normalizing flows. The accuracy and efficiency of our approach are demonstrated in the calculations of a large number of vibrational states of the triatomic H$_2$S molecule as well as ground and several excited electronic states of prototypical one-electron systems including the hydrogen atom, the molecular hydrogen ion, and a carbon atom in a single-active-electron approximation. The results demonstrate significant improvements in the accuracy of energy predictions and accelerated basis-set convergence even when using normalizing flows with a small number of parameters. The present approach can be also seen as the optimization of a set of intrinsic coordinates that best capture the underlying physics within the given basis set.

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Contributing Institute(s):

1. CFEL-CMI (FS-CFEL-CMI)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. HIDSS-0002 - DASHH: Data Science in Hamburg - Helmholtz Graduate School for the Structure of Matter (2019_IVF-HIDSS-0002) (2019_IVF-HIDSS-0002)
3. DFG project 390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
4. DFG project 194651731 - EXC 1074: Hamburger Zentrum für ultraschnelle Beobachtung (CUI): Struktur, Dynamik und Kontrolle von Materie auf atomarer Skala (194651731) (194651731)

Experiment(s):

1. No specific instrument

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Database coverage:
Published

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Linked articles:

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Journal Article Fernandez Corral, A.CFEL*DESY* ; Vogt, E.DESY* ; Iske, A.CFEL*Extern* ; Saleh, Y. (Corresponding author)CFEL*DESY* ; Küpper, J.CFEL*XFEL.EU*DESY* ; Yachmenev, A. (Corresponding author)CFEL*DESY*
Computing Excited States of Molecules Using Normalizing Flows
Journal of chemical theory and computation 21(10), 5221 - 5229 (2025) [10.1021/acs.jctc.5c00590]2025     Files  Fulltext by arXiv.org BibTeX | EndNote: XML, Text | RIS

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