Probing anomalous relaxation by coherent multidimensional optical spectroscopy
Abstract
We propose to study the origin of algebraic decay of two-point correlation functions observed in glasses, proteins, and quantum dots by their nonlinear response to sequences of ultrafast laser pulses. Power-law spectral singularities and temporal relaxation in two-dimensional correlation spectroscopy (2DCS) signals are predicted for a continuous time random walk model of stochastic spectral jumps in a two level system with a power-law distribution of waiting times (t) t-α -1. Spectroscopic signatures of stationary ensembles for 1<α <2 and aging effects in nonstationary ensembles with 0<α <1 are identified.
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