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]

This record in other databases:      

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

Report No.: arXiv:2308.16468

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.

---

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. 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

Appears in the scientific report 2025

---

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

---

---

Linked articles:

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Preprint 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*
Computing excited states of molecules using normalizing flows
    Files  Fulltext by arXiv.org BibTeX | EndNote: XML, Text | RIS

---