Abstract Exact equations for correlation energy and kinetic energy correction functionals are derived in the time‐dependent density functional theory. Hierarchies of equations are also obtained and approximate functionals are proposed by truncation of the hierarchies at different orders. Explicit relations for the correlation energy and its kinetic component along the adiabatic path are given in terms of powers of the moments of the electron density. © 2003 Wiley Periodicals, Inc. Int J Quantum Chem, 2003
Exact time-dependent density-functional theory (DFT) separates the exchange-correlation potential into interaction and kinetic-correlation components, but the structural relation between them remains unclear. We establish a representability constraint based on the off-diagonal expansion of the one-electron reduced density matrix (1RDM) relative to a chosen reference dynamics. A non-zero linear off-diagonal term of the 1RDM generates a current density beyond the representable space of the reference, while a nontrivial quadratic off-diagonal structure activates the kinetic-correlation component. The resulting hierarchy provides a criterion for assessing, from the spatial locality of electronic correlation, whether a given exchange-correlation functional or a more general electron-correlation approximation remains adequate. In a one-dimensional two-electron correlation quench, retaining the exact interaction component while setting the kinetic component to zero suppresses the density broadening of the exact evolution. These results establish a spatial-order hierarchy among the force components governing the density dynamics and provide an exact constraint for the construction and assessment of nonadiabatic approximations.
In this paper we derive the evolution equations for non-Markovian multiple-time correlation functions of an open quantum system without using any approximation. We find that these equations conform an open hierarchy in which
N-time correlation functions are dependent on
(N+1)-time correlations. This hierarchy of equations is consistently obtained with two different methods: A first one based on Heisenberg equations of system operators, and a second one based on system propagators. The dependency on higher order correlations, and therefore the open hierarchy structure, only disappears in certain particular cases and when some hypothesis or approximations are considered in the equations. In this paper we consider a perturbative approximation and derive the general evolution equation for
N-time correlations. This equation turns to depend only on
N-time and lower order correlation functions, conforming a closed hierarchy structure that is useful for computational purposes.