A reformulation of time-dependent Kohn-Sham theory in terms of the second time derivative of the density (2012.04953v1)

Abstract: The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation potential as an implicit density functional. It is shown that this suggests a reformulation of TDDFT in terms of the second time derivative of the density, rather than the density itself. The result is a time-local Kohn-Sham scheme of second order in time whose causal structure is more transparent than that of the usual Kohn-Sham formalism. The scheme can be used to construct new approximations at the exchange-only level and beyond, and it offers a straightforward definition of the exact adiabatic approximation.