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Electronic absorption spectra from off-diagonal quantum master equations.
- Source :
- Journal of Chemical Physics; 9/14/2022, Vol. 157 Issue 10, p1-10, 10p
- Publication Year :
- 2022
-
Abstract
- Quantum master equations (QMEs) provide a general framework for describing electronic dynamics within a complex molecular system. Off-diagonal QMEs (OD-QMEs) correspond to a family of QMEs that describe the electronic dynamics in the interaction picture based on treating the off-diagonal coupling terms between electronic states as a small perturbation within the framework of second-order perturbation theory. The fact that OD-QMEs are given in terms of the interaction picture makes it non-trivial to obtain Schrödinger picture electronic coherences from them. A key experimental quantity that relies on the ability to obtain accurate Schrödinger picture electronic coherences is the absorption spectrum. In this paper, we propose using a recently introduced procedure for extracting Schrödinger picture electronic coherences from interaction picture inputs to calculate electronic absorption spectra from the electronic dynamics generated by OD-QMEs. The accuracy of the absorption spectra obtained this way is studied in the context of a biexciton benchmark model, by comparing spectra calculated based on time-local and time-nonlocal OD-QMEs to spectra calculated based on a Redfield-type QME and the non-perturbative and quantum-mechanically exact hierarchical equations of motion method. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00219606
- Volume :
- 157
- Issue :
- 10
- Database :
- Complementary Index
- Journal :
- Journal of Chemical Physics
- Publication Type :
- Academic Journal
- Accession number :
- 159105194
- Full Text :
- https://doi.org/10.1063/5.0106888