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J Chem Phys. 2006 Aug 28;125(8):084502.

Characterization of spectral diffusion from two-dimensional line shapes.

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1
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.

Abstract

The analysis of line shapes in two-dimensional optical and infrared spectroscopies is a powerful approach to characterizing the dynamics of molecules in the condensed phase. Changes in line shape from diagonally elongated to symmetric as a function of waiting time arise from evolution of the transition frequency. We describe a number of quantitative measures of frequency fluctuations and spectral diffusion through the analysis of two-dimensional (2D) line shapes. These metrics are identical to the system's frequency correlation function and independent of population relaxation in the limit of a short time approximation for the 2D response. We also test the broader applicability of these expressions for analyzing three-level vibrational systems and experiments with finite pulses.

PMID:
16965024
DOI:
10.1063/1.2232271
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