Theory of Excitation Broadening Using Time-Dependent Density Functional Theory for Open Quantum Systems
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CitationTempel, David G., and Alán Aspuru-Guzik. Forthcoming. Theory of excitation broadening using time-dependent density functional theory for open quantum systems.
AbstractThe Casida equations of linear response TDDFT are extended to calculate linear spectra of open quantum systems evolving according to a Markovian master equation. By mapping a many-body open quantum system onto an open, non-interacting Kohn-Sham system, extrinsic line broadening due to electron-bath coupling can be described exactly within TDDFT. The structure of the resulting matrix equations are analyzed for the generic case of electrons linearly coupled to a harmonic bath within Redfield theory. An approximate form of the exchange-correlation kernel based on first-order G\"orling-Levy perturbation theory is derived.
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