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Title: Linear and third- and fifth-order nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration

We study hole, electron, and exciton transports in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third-, and fifth-order nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole, and exciton transfers can lead to non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional (2D) spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.
Authors:
 [1] ;  [2]
  1. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  2. Department of Chemistry, Kyoto University, Kyoto (Japan)
Publication Date:
OSTI Identifier:
22415898
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; CORRELATIONS; COUPLING; ELECTRON SPECTRA; ELECTRON SPECTROSCOPY; ELECTRONS; EQUATIONS OF MOTION; EXCITED STATES; EXCITONS; HOLES; NONLINEAR PROBLEMS; OSCILLATORS; SPECTRAL DENSITY; TWO-DIMENSIONAL SYSTEMS