Response-theory for nonresonant hole burning: Stochastic dynamics

Abstract

Using non-linear response theory the time signals relevant for nonresonant spectral hole burning are calculated. The step-reponse function following the application of a high amplitude ac field (pump) and an intermediate waiting period is shown to be the sum of the equilibrium integrated response and a modification due to the preparation via ac irradiation. Both components are calculated for a class of stochastic dipole reorientation models. The results indicate that the method can be used for a clearcut distinction of homogeneously and heterogeneously broadened susceptibilities as they occur in the relaxation of supercooled liquids or other disordered materials. This is because only in the heterogeneous case is a frequency selective modification of the response possible.