Excited state quantum-classical molecular dynamics

We are focusing on developing a predictive theoretical, algorithmic and computational framework describing the many-body dynamics of the plasma–wall interactions by applying multiscale quantum-classical (QC) molecular dynamics (MD) and quantum chemistry approaches. Computer simulations of the dynamics of molecular systems often encounter serious limitations, of both phenomenological and quantitative nature, due to our inability to treat non-adiabatic transition dynamics and evolution beyond the ground Born–Oppenheimer electronic surface. This is, in particular, present due to charge transfer, collisional-cascade excitations and chemical sputtering of plasma ions impinging on a plasma-facing surface. A quantum mechanical treatment of the full non-adiabatic multibody dynamics is not currently feasible. To address existing deficiencies in knowledge of non-adiabatic MD, we propose excited state many-body dynamics by considering multiphysics described by time-dependent versions of the mean-field theories as well as QC Liouville equations, combined with multiresolution techniques for solving the quantum part of the problem.

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