Using iterative evaluation of the real-time path integral expression, we calculate four-time correlation functions for one-dimensional systems coupled to model dissipative environments. We use these correlation functions to calculate response functions relevant to third order infrared or seventh order Raman experiments for harmonic, Morse, and quadratic-quartic potentials interacting with harmonic and two-level-system dissipative baths. Our calculations reveal the role of potential features (anharmonicity and eigenvalue spectrum), both on short and long time scales, on the response function. Further, thermal excitation causes dramatic changes in the appearance of the response function, introducing symmetry with respect to the main diagonal. Finally, coupling to harmonic dissipative baths leads to decay of the response function (primarily along the direction) and a broadening of the peaks in its Fourier transform. At high temperatures two-level-system baths are less efficient in destroying coherence than harmonic baths of similar parameters.
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7 April 2010
Research Article|
April 02 2010
Multitime response functions and nonlinear spectra for model quantum dissipative systems
Mohammad M. Sahrapour;
Mohammad M. Sahrapour
1Department of Physics,
University of Illinois
, Urbana, Illinois 61801, USA
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Nancy Makri
Nancy Makri
a)
1Department of Physics,
University of Illinois
, Urbana, Illinois 61801, USA
2Department of Chemistry,
University of Illinois
, Urbana, Illinois 61801, USA
Search for other works by this author on:
a)
Electronic mail: nancy@makri.scs.uiuc.edu.
J. Chem. Phys. 132, 134506 (2010)
Article history
Received:
June 12 2009
Accepted:
February 08 2010
Citation
Mohammad M. Sahrapour, Nancy Makri; Multitime response functions and nonlinear spectra for model quantum dissipative systems. J. Chem. Phys. 7 April 2010; 132 (13): 134506. https://doi.org/10.1063/1.3336463
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