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 $\psi (t)\sim t^{-\alpha -1}$. Spectroscopic signatures of stationary ensembles for $1<\alpha <2$ and aging effects in nonstationary ensembles with $0<\alpha <1$ are identified.