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Quantitative agreement between experiment and theory for Vibrational Circular Dichroism enhanced by electronically excited states

2025/06/19 by Mariia Sapova, Sapova, Mariia, Chandan Kumar +7
Chemistry · Neuroscience · Physics and Astronomy · #Advanced Chemical Physics Studies #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Molecular spectroscopy and chirality #Photoreceptor and optogenetics research

paper · pdf · doi:10.48550/arxiv.2506.16270

openalex publication_date 2025/06/19 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28

Abstract

Intensity enhancement in vibrational circular dichroism (VCD) arises in open-shell transition metal complexes from coupling between low-lying excited states (LLESs) and ground-state vibrational modes. In this work we apply Nafie's vibronic coupling theory to M(II)-(-)-sparteine-Cl2 to investigate these enhancement effects. We show that the VCD intensity is extremely sensitive to the excitation energies that neither time-dependent density functional theory (TDDFT) nor state-averaged complete active space self consistent field (SA-CASSCF) calculations can predict with sufficient accuracy. We argue that instead of using more accurate quantum chemistry methods these excitation energies can be treated as parameters and optimized against experimental spectra. With this approach we obtain simulated VCD similarity scores above 0.4, a threshold considered reliable for absolute configuration assignment.

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