In this paper, we present a quantum stochastic model for spectroscopic lineshapes 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 differences in the predicted lineshapes, notably in terms of asymmetry, and variation with the increasing background population.
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21 October 2020
Research Article|
October 21 2020
Stochastic scattering theory for excitation-induced dephasing: Comparison to the Anderson–Kubo lineshape
Special Collection:
Excitons: Energetics and Spatio-temporal Dynamics
Hao Li
;
Hao Li
1
Department of Chemistry, University of Houston
, Houston, Texas 77204, USA
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Ajay Ram Srimath Kandada
;
Ajay Ram Srimath Kandada
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
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Carlos Silva
;
Carlos Silva
3
School of Chemistry and Biochemistry, Georgia Institute of Technology
, 901 Atlantic Drive, Atlanta, Georgia 30332, USA
4
School of Physics, Georgia Institute of Technology
, 837 State Street, Atlanta, Georgia 30332, USA
5
School of Materials Science and Engineering, Georgia Institute of Technology
, North Avenue, Atlanta, Georgia 30332, USA
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Eric R. Bittner
Eric R. Bittner
a)
1
Department of Chemistry, University of Houston
, Houston, Texas 77204, USA
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Excitons: Energetics and Spatio-temporal Dynamics.
J. Chem. Phys. 153, 154115 (2020)
Article history
Received:
August 24 2020
Accepted:
September 29 2020
Citation
Hao Li, Ajay Ram Srimath Kandada, Carlos Silva, Eric R. Bittner; Stochastic scattering theory for excitation-induced dephasing: Comparison to the Anderson–Kubo lineshape. J. Chem. Phys. 21 October 2020; 153 (15): 154115. https://doi.org/10.1063/5.0026467
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