Jump to main content
Jump to site search

Issue 26, 2018
Previous Article Next Article

An ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules

Author affiliations

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.

Graphical abstract: An ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules

Back to tab navigation

Publication details

The article was received on 11 Apr 2018, accepted on 24 May 2018 and first published on 19 Jun 2018


Article type: Paper
DOI: 10.1039/C8CP02321B
Phys. Chem. Chem. Phys., 2018,20, 17762-17772
  • Open access: Creative Commons BY license
  •   Request permissions

    An ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules

    V. M. Freixas, S. Fernandez-Alberti, D. V. Makhov, S. Tretiak and D. Shalashilin, Phys. Chem. Chem. Phys., 2018, 20, 17762
    DOI: 10.1039/C8CP02321B

    This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material.

    Reproduced material should be attributed as follows:

    • For reproduction of material from NJC:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the Centre National de la Recherche Scientifique (CNRS) and the RSC.
    • For reproduction of material from PCCP:
      [Original citation] - Published by the PCCP Owner Societies.
    • For reproduction of material from PPS:
      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
    • For reproduction of material from all other RSC journals:
      [Original citation] - Published by The Royal Society of Chemistry.

    Information about reproducing material from RSC articles with different licences is available on our Permission Requests page.

Search articles by author

Spotlight

Advertisements