Institute of Theoretical Physics · Faculty of Mathematics and Physics, Charles University
J. Phys. Chem. C 111(32), 11970-11981 (2007)
A method to describe the quantum dynamics of photoinduced heterogeneous electron-transfer processes at dye-semiconductor interfaces is proposed. The method is based on a model Hamiltonian, the parameters of which are determined by first-principles electronic structure calculations and a partitioning scheme to define localized donor and acceptor states as well as donor-acceptor coupling matrix elements. On the basis of this modeling procedure, accurate quantum dynamical simulations are performed employing the multilayer multiconfiguration time-dependent Hartree method. As a representative example, applications to coumarin 343 adsorbed on titanium oxide nanoparticles are presented. The results of the simulations show that the ultrafast electron-injection process in this system is accompanied by electronic coherence effects, which are partially quenched due to electronic-nuclear coupling.
@article{UTF63,
author = {Kondov, I. and Čížek, M. and Benesch, C. and Wang, H. B. and Thoss, M.},
title = {{Quantum dynamics of photoinduced electron-transfer reactions in dye-semiconductor systems: First-principles description and application to coumarin 343-TiO2}},
journal = {J. Phys. Chem. C},
publisher = {AMER CHEMICAL SOC},
address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA},
volume = {111},
number = {32},
pages = {11970-11981},
year = {2007},
url = {http://utf.mff.cuni.cz/\textasciitilde{}cizek/naseclanky/2007\_kcbwt.pdf},
}