Photoinduced processes in extended molecular systems are often ultrafast and involve strong electron-vibration (vibronic) coupling effects which necessitate a non-perturbative treatment. In the approach presented here, high-dimensional vibrational subspaces are expressed in terms of effective modes, and hierarchical chains of such modes which sequentially resolve the dynamics as a function of time. This permits introducing systematic reduction procedures, both for discretized vibrational distributions and for continuous distributions characterized by spectral densities. In the latter case, a sequence of spectral densities is obtained from a Mori/Rubin-type continued fraction representation. The approach is suitable to describe nonadiabatic processes at conical intersections, excitation energy transfer in molecular aggregates, and related transport phenomena that can be described by generalized spin-boson models.
Hierarchical Effective-Mode Approach for Extended Molecular Systems / R. Martinazzo, K.H. Hughes, I. Burghardt - In: Advances in the Theory of Quantum Systems in Chemistry and Physics / [a cura di] P.E.E. Hoggan, E.J.J. Brändas, J. Maruani, P. Piecuch and G. Delgado-Barrio. - [s.l] : Springer, 2012. - ISBN 978-94-007-2075-6. - pp. 269-283 [10.1007/978-94-007-2076-3_15]
Hierarchical Effective-Mode Approach for Extended Molecular Systems
R. MartinazzoPrimo
;
2012
Abstract
Photoinduced processes in extended molecular systems are often ultrafast and involve strong electron-vibration (vibronic) coupling effects which necessitate a non-perturbative treatment. In the approach presented here, high-dimensional vibrational subspaces are expressed in terms of effective modes, and hierarchical chains of such modes which sequentially resolve the dynamics as a function of time. This permits introducing systematic reduction procedures, both for discretized vibrational distributions and for continuous distributions characterized by spectral densities. In the latter case, a sequence of spectral densities is obtained from a Mori/Rubin-type continued fraction representation. The approach is suitable to describe nonadiabatic processes at conical intersections, excitation energy transfer in molecular aggregates, and related transport phenomena that can be described by generalized spin-boson models.
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