Extended quantum jump description of vibronic two-dimensional spectroscopy.

J Chem Phys

Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Campus Nord, Emil-Fischer-St. 42, 97074 Würzburg, Germany.

Published: June 2015

We calculate two-dimensional (2D) vibronic spectra for a model system involving two electronic molecular states. The influence of a bath is simulated using a quantum-jump approach. We use a method introduced by Makarov and Metiu [J. Chem. Phys. 111, 10126 (1999)] which includes an explicit treatment of dephasing. In this way it is possible to characterize the influence of dissipation and dephasing on the 2D-spectra, using a wave function based method. The latter scales with the number of stochastic runs and the number of system eigenstates included in the expansion of the wave-packets to be propagated with the stochastic method and provides an efficient method for the calculation of the 2D-spectra.

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http://dx.doi.org/10.1063/1.4919870DOI Listing

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