Solvation beyond the linear response regime

Transient two-dimensional infrared spectroscopy (2D-IR) on a charge transfer model system is used as a nonlinear probe of solvation dynamics. Unlike what is expected in the linear response case, nonequilibrium relaxation and equilibrium spectral diffusion occur on different time scales. Transient 2D...

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Bibliographic Details
Published in:Physical review letters 2005-08, Vol.95 (8), p.083201-083201, Article 083201
Main Authors: BREDENBECK, Jens, HELBING, Jan, HAMM, Peter
Format: Article
Language:English
Subjects:
Atomic and molecular collision processes and interactions
Atomic and molecular physics
Charge transfer
Exact sciences and technology
Physics
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Summary:Transient two-dimensional infrared spectroscopy (2D-IR) on a charge transfer model system is used as a nonlinear probe of solvation dynamics. Unlike what is expected in the linear response case, nonequilibrium relaxation and equilibrium spectral diffusion occur on different time scales. Transient 2D-IR spectroscopy is shown to be sensitive to higher order frequency fluctuation correlation functions, and provides evidence for a coupling between commonly observed fast and slow solvation processes.
ISSN:0031-9007
1079-7114
DOI:10.1103/PhysRevLett.95.083201