Article (Scientific journals)
Multidimensional Quantum Mechanical Modeling of Electron Transfer and Electronic Coherence in Plant Cryptochromes: The Role of Initial Bath Conditions
Mendive-Tapia, David; Mangaud, Etienne; Firmino, Thiago et al.
2018In Journal of Physical Chemistry B, 122, p. 126-136
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Keywords :
electron transfer; quantum coherence; MCTDH
Abstract :
[en] A multidimensional quantum mechanical protocol is used to describe the photoinduced electron transfer and electronic coherence in plant cryptochromes without any semiempirical, e.g., experimentally obtained, parameters. Starting from a two-level spin-boson Hamiltonian we look at the effect that the initial photoinduced nuclear bath distribution has on an intermediate step of this biological electron transfer cascade for two idealized cases. The first assumes a slow equilibration of the nuclear bath with respect to the previous electron transfer step that leads to an ultrafast decay with little temperature dependence; while the second assumes a prior fast bath equilibration on the donor potential energy surface leading to a much slower decay, which contrarily displays a high temperature dependence and a better agreement with previous theoretical and experimental results. Beyond Marcus and semiclassical pictures these results unravel the strong impact that the presence or not of equilibrium initial conditions has on the electronic population and coherence dynamics at the quantum dynamics level in this and conceivably in other biological electron transfer cascades.
Disciplines :
Chemistry
Author, co-author :
Mendive-Tapia, David;  Theoretische Chemie, heidelberg
Mangaud, Etienne
Firmino, Thiago
de la Lande, Aurélien
Desouter, Michèle ;  Université de Liège - ULiège > Département de chimie (sciences) > Département de chimie (sciences)
Meyer, Hans-Dieter
Gatti, Fabien
Language :
English
Title :
Multidimensional Quantum Mechanical Modeling of Electron Transfer and Electronic Coherence in Plant Cryptochromes: The Role of Initial Bath Conditions
Publication date :
2018
Journal title :
Journal of Physical Chemistry B
ISSN :
1520-6106
eISSN :
1520-5207
Publisher :
American Chemical Society, United States - District of Columbia
Volume :
122
Pages :
126-136
Peer reviewed :
Peer Reviewed verified by ORBi
Available on ORBi :
since 16 April 2018

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