Understanding the fundamental connection between electronic correlation and decoherence
arXiv:1506.01433 · doi:10.1021/acs.jpclett.6b00467
Abstract
We introduce a theory that exposes the fundamental and previously overlooked connection between the correlation among electrons and the degree of quantum coherence of electronic states in matter. For arbitrary states, the effects only decouple when the electronic dynamics induced by the nuclear bath is pure-dephasing in nature such that , where is the electronic Hamiltonian and is the electron-nuclear coupling. We quantitatively illustrate this connection via exact simulations of a Hubbard-Holstein molecule using the Hierarchical Equations of Motion that show that increasing the degree of electronic interactions can enhance or suppress the rate of electronic coherence loss.
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