We introduce a theory that exposes the fundamental 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 of pure-dephasing nature such that [HS,HSB]=0, where HS is the electronic Hamiltonian and HSB is the electron-nuclear coupling. We quantitatively illustrate this connection via numerically exact simulations of a Hubbard-Holstein molecule using the Hierarchical Equation of Motion approach that show that increasing the degree of electronic interactions can enhance or suppress the rate of electronic coherence loss.

Understanding the fundamental connection between electronic correlation and decoherence

251st National Meeting (2016)

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