In this paper, I will present a multistate density functional theory (MSDFT) in the framework of valence bond (VB) theory for study of chemical reactions, including proton coupled electron transfer (PCET) processes.  The method is based on non-orthogonal, block-localized molecular orbital (BLMO) and block-localized density functional theory (BLDFT), in which localized electronic configurations, called diabatic states, are obtained by construction with specific orbital and charge constraints. A key feature of MSDFT is that the electron density of the adiabatic ground state is not directly computed nor used to obtain the ground-state energy. Rather, the ground-state energy is determined by diagonalization of the VB Hamiltonian. This represents a departure from the standard single-determinant Kohn-Sham density functional theory. The methods of MSDFT and BLDFT are illustrated by applications tochemical and PCET reactions.

Unified quantum mechanical approach to macromolecular simulations: From a single electron to fully solvated proteins.

241st National Meeting (2011)

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