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Phys. Chem. Chem. Phys., 2009, 11, 4509 - 4522, DOI: 10.1039/b903064f

Time-dependent current-density functional theory for generalized open quantum systems

Joel Yuen-Zhou, César Rodríguez-Rosario and Alán Aspuru-Guzik

In this article, we prove the one-to-one correspondence between vector potentials and particle and current densities in the context of master equations with arbitrary memory kernels, therefore extending time-dependent current-density functional theory (TD-CDFT) to the domain of generalized many-body open quantum systems (OQS). We also analyse the issue of A-representability for the Kohn–Sham (KS) scheme proposed by DAgosta and Di Ventra for Markovian OQS [Phys. Rev. Lett. 2007, 98, 226403] and discuss its domain of validity. We suggest ways to expand their scheme, but also propose a novel KS scheme where the auxiliary system is both closed and non-interacting. This scheme is tested numerically with a model system, and several considerations for the future development of functionals are indicated. Our results formalize the possibility of practising TD-CDFT in OQS, hence expanding the applicability of the theory to non-Hamiltonian evolutions.

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