Journal Article

PUBDB-2023-05096

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Computing Excited States of Molecules Using Normalizing Flows

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*

2025
[Verlag nicht ermittelbar]

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Please use a persistent id in citations: doi:10.1021/acs.jctc.5c00590  doi:10.3204/PUBDB-2023-05096

Abstract: Calculations of highly excited and delocalizedmolecular vibrational states are computationally challenging tasks,which strongly depend on the choice of coordinates for describingvibrational motions. We introduce a new method that leveragesnormalizing flows, i.e, parametrized invertible functions, to learnoptimal vibrational coordinates that satisfy the variational principle.This approach produces coordinates tailored to the vibrational problem at hand, significantly increasing the accuracy and enhancingthe basis set convergence of the calculated energy spectrum. The efficiency of the method is demonstrated in calculations of the 100lowest excited vibrational states of H$_2$S, H$_2$CO, and HCN/HNC. The method effectively captures the essential vibrational behaviorof molecules by enhancing the separability of the Hamiltonian and hence allows for an effective assignment of approximate quantumnumbers. We demonstrate that the optimized coordinates are transferable across different levels of basis set truncation, enabling acost-efficient protocol for computing vibrational spectra of high-dimensional systems.

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Contributing Institute(s):

1. CFEL-CMI (FS-CFEL-CMI)
2. beauftragt von UNI (UNI/CUI)
3. Uni Hamburg / Experimentalphysik (UNI/EXP)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. AIM, DFG project G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
3. HIDSS-0002 - DASHH: Data Science in Hamburg - Helmholtz Graduate School for the Structure of Matter (2019_IVF-HIDSS-0002) (2019_IVF-HIDSS-0002)
4. Quantum-mechanical modeling of the dissociation of hydrogen bonds (101155136) (101155136)

Experiment(s):

1. No specific instrument

Appears in the scientific report 2025

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Electronics and Telecommunications Collection ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 5 ; JCR ; Nationallizenz ; SCOAP3 sponsored Journal ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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