Freixas, VM, Fernandez-Alberti, S, Makhov, DV et al. (2 more authors) (2018) An ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules. Physical Chemistry Chemical Physics, 20 (26). pp. 17762-17772. ISSN 1463-9076
Abstract
We present a new implementation of the Ab Initio Multiple Cloning (AIMC) method, which is applied for non-adiabatic excited-state molecular dynamics simulations of photoinduced processes in conjugated molecules. Within our framework, the multidimensional wave-function is decomposed into a superposition of a number of Gaussian coherent states guided by Ehrenfest trajectories that are suited to clone and swap their electronic amplitudes throughout the simulation. New generalized cloning criteria are defined and tested. Because of sharp changes of the electronic states, which are common for conjugated polymers, the electronic parts of the Gaussian coherent states are represented in the Time Dependent Diabatic Basis (TDDB). The input to these simulations in terms of the excited-state energies, gradients and non-adiabatic couplings, is calculated on-the-fly using the Collective Electron Oscillator (CEO) approach. As a test case, we consider the photoinduced unidirectional electronic and vibrational energy transfer between two- and three-ring linear poly(phenylene ethynylene) units linked by meta-substitution. The effects of the cloning procedure on electronic and vibrational coherence, relaxation and unidirectional energy transfer between dendritic branches are discussed.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | (c) the Owner Societies 2018. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. (https://creativecommons.org/licenses/by/3.0/) |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemistry (Leeds) > Physical Chemistry (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 30 May 2018 15:12 |
Last Modified: | 25 Jun 2023 21:21 |
Status: | Published |
Publisher: | Royal Society of Chemistry (RSC) |
Identification Number: | 10.1039/C8CP02321B |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:131351 |