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.

References in corpus (4)

• Statistical Aging and Non Ergodicity in the Fluorescence of Single Nanocrystals
• Lineshape Theory and Photon Counting Statistics for Spectral Fluctuations in Quantum Dots: a Lévy Walk Process
• Linear response to perturbation of non-exponential renewal processes
• Absorption and Emission in the non-Poisson case

Cited by in corpus (4)

• Asymptotically exact theory for nonlinear spectroscopy of random quantum magnets
• Anomalous Lineshapes and Aging Effects in Two-Dimensional Correlation Spectroscopy
• Simulations of coherent nonlinear optical response of molecular vibronic dimers
• Interplay between Static and Dynamic Disorder: Contrasting Effects on Dark State Population inside a Cavity