Stochastic scattering theory for excitation induced dephasing: Comparison to the Anderson-Kubo lineshape

Abstract

In this paper we present a quantum stochastic model for spectroscopic line-shapes in the presence of a co-evolving and non-stationary 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. Itô's Lemma then allows us to easily construct and evaluate correlation functions and response functions. Focusing on the linear response, we compare our model to the classic Anderson-Kubo model. While similar in motivation, there are profound differences in the predicted lineshapes, notably in terms of asymmetry, and variation with increasing background population.

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Cited by in corpus (7)

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• Homogeneous optical linewidths in hybrid Ruddlesden-Popper metal halides can only be measured using nonlinear spectroscopy
• The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
• Many-Exciton Quantum Dynamics in a Ruddlesden-Popper Tin Iodide
• Quantum decoherence dynamics in stochastically fluctuating environments
• Stochastic exciton-scattering theory of optical lineshapes: Renormalized many-body contributions
• Excitons: Energetics and spatio-temporal dynamics