The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering

Author:

Li Hao1,Shah S.A.1,Kandada Ajay Ram Srimath2,Silva Carlos3,Piryatinski Andrei4,Bittner Eric R.1

Affiliation:

1. Department of Chemistry, University of Houston, Houston, Texas, USA;

2. Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, North Carolina, USA

3. School of Chemistry and Biochemistry, School of Physics, and School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia, USA

4. Theoretical Division, Los Alamos National Laboratory, Los Alamos, New Mexico, USA

Abstract

We review our recent quantum stochastic model for spectroscopic lineshapes in the presence of a coevolving and nonstationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein–Uhlenbeck process. Here, we present an overview of the theoretical techniques we have developed as applied to predicting coherent nonlinear spectroscopic signals. We show how direct (Coulomb) and exchange coupling to the bath give rise to distinct spectral signatures and discuss mathematical limits on inverting spectral signatures to extract the background density of states.

Publisher

Annual Reviews

Subject

Physical and Theoretical Chemistry

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