Non-equilibrium electron-vibrational dynamics at finite temperature determines key coherence properties of molecular systems in quantum information science. I apply thermo-field theory on the Keldysh contour to incorporate vibronic interactions in density functional theory and correlated electronic structure methods. I outline the treatment of non-Markovian effects and demonstrate the emergence of Markovian limits of open quantum system dynamics in the new theory. I apply the new method to simulate the spin-coherence and spin-optical dynamics of molecular and solid-state qubits with quantum sensing and quantum communication applications and study the influence of temperature and symmetry on the coherence properties of these systems. The combination of method development and application offers new insight into the quantum dynamics of spin qubits and enables the engineering of quantum states for quantum technology applications.

<i>Ab initio</i> quantum chemistry methods for coupled electron-vibrational dynamics

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ACS Fall 2022

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Ab initio quantum chemistry methods for coupled electron-vibrational dynamics