Phys. Rev. Lett. 95, 083201 (2005) [4 pages]Solvation beyond the Linear Response RegimeReceived 17 September 2004; published 18 August 2005 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. © 2005 The American Physical Society URL:
http://link.aps.org/doi/10.1103/PhysRevLett.95.083201
DOI:
10.1103/PhysRevLett.95.083201
PACS:
34.10.+x, 34.70.+e, 78.47.+p, 82.53.Uv
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