Using Adiabatic Energy Splitting To Compute Dexter Energy Transfer Couplings.

ABSTRACT

Dexter energy transfer and transport (DET) are of broad interest in energy science, and DET rates depend on electronic couplings between donor and acceptor species. DET couplings are challenging to compute since they originate from both one- and two-particle interactions, and the strength of this interaction drops approximately exponentially with donor-acceptor distances. Using adiabatic energy splitting to compute DET couplings has advantages because adiabatic states can be calculated directly using conventional quantum chemical methods. We describe a minimum energy splitting method to compute the DET coupling by altering molecular geometries to drive the systems into a T1/T2 energy quasi-degenerate-activated DA complex. We explore the accuracy of various quantum chemical approaches to calculate the Dexter couplings.