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The Role of Vibronic Coupling in the Electronic Spectroscopy of Maleimide: A Multi-Mode and Multi-State Quantum Dynamics Study

Lehr, A; Gomez Rodriguez, S; Parkes, MA; Worth, G; (2020) The Role of Vibronic Coupling in the Electronic Spectroscopy of Maleimide: A Multi-Mode and Multi-State Quantum Dynamics Study. Physical Chemistry Chemical Physics 10.1039/d0cp04514d. (In press). Green open access

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Abstract

The first two excitation bands below 7 eV in the electronic absorption spectrum of maleimide are investigated using a model Hamiltonian including four low-lying singlet excited states within the manifold of 24 vibrational modes. The role of non-adiabatic effects is studied and shines light on both the broad, inter-state coupling–dominated spectral band as well as the fine-structured, not-so-strong coupled band. Calculations have been performed using the Multiconfigurational Time-Dependent Hartree (MCTDH) wavepacket propagation method as well as its multilayer version (ML-MCTDH) using a quadratic vibronic coupling (QVC) Hamiltonian model where parameters are obtained from fitting adiabatic potential energy surfaces computed by ab initio methods. The quantum dynamics calculations provide information on the relaxation dynamics and the vibrational modes involved. Already with a low-order vibronic coupling model and only a few modes being considered, a quantitative agreement with the experimental spectrum is obtained. However, it is found that all modes need to be considered to get a full picture of the photo-excited relaxation dynamics of this molecule.

Type: Article
Title: The Role of Vibronic Coupling in the Electronic Spectroscopy of Maleimide: A Multi-Mode and Multi-State Quantum Dynamics Study
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/d0cp04514d
Publisher version: https://doi.org/10.1039/D0CP04514D
Language: English
Additional information: © the Owner Societies 2020. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence (http://creativecommons.org/licenses/by-nc/3.0/).
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10113315
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