Related papers: Fundamentals of Time-Resolved Charge-Transfer in T…
Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…
The time-dependent exchange-correlation potential has an unusual task in directing fictitious non-interacting electrons to move with exactly the same probability density as true interacting electrons. This has intriguing implications for…
Long-range charge-transfer excitations pose a major challenge for time-dependent density functional approximations. We show that spin-symmetry-breaking offers a simple solution for molecules composed of open-shell fragments, yielding…
Adiabatic time-dependent density functional theory fails for excitations of a heteroatomic molecule composed of two open-shell fragments at large separation. Strong frequency-dependence of the exchange-correlation kernel is necessary for…
We show that the exact exchange-correlation potential of time-dependent density-functional theory displays dynamical step structures that have a spatially non-local and time non-local dependence on the density. Using one-dimensional…
We identify peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory that are crucial for time-resolved electron scattering in a model one-dimensional system. These structures are…
Long-range charge transfer excited states are notoriously badly underestimated in time-dependent density functional theory (TDDFT). We resolve how {\it exact} TDDFT captures charge transfer between open-shell species: in particular the role…
It was recently shown [Y. Suzuki, L. Lacombe, K. Watanabe, and N. T. Maitra, Phys. Rev. Lett. 119, 263401 (2017)] that peak and valley structures in the exact exchange-correlation potential of time-dependent density functional theory are…
We show that an asymmetric two-fermion two-site Hubbard model illustrates the essential features of long-range charge-transfer dynamics in a real-space molecule. We apply a resonant field that transfers one fermion from one site to the…
It has been known for some time that the exchange-correlation potential in time-dependent density functional theory is an intrinsically nonlocal functional of the density as soon as one goes beyond the adiabatic approximation. In this paper…
A fundamental property of a quantum system driven by an external field is that when the field is turned off the positions of its response frequencies are independent of the time at which the field is turned off. We show that this leads to…
We employ the density matrix renormalization group to construct the exact time-dependent exchange correlation potential for an impurity model with an applied transport voltage. Even for short-ranged interaction we find an infinitely…
We explore an asymmetric two-fermion Hubbard dimer to test the accuracy of the adiabatic approximation of time-dependent density functional theory in modelling time-resolved charge transfer. We show that the model shares essential features…
We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…
We identify the key property that the exchange-correlation (XC) kernel of time-dependent density functional theory must have in order to describe long-range charge-transfer excitations. We show that the discontinuity of the XC potential as…
We investigate an extension of excited state mean-field theory in which the energy expression is augmented with density functional components in an effort to include the effects of weak electron correlations. The approach remains…
We perform model calculations for a stretched LiF molecule, demonstrating that nonadiabatic charge transfer effects can be accurately and seamlessly described within a density functional framework. In alkali halides like LiF, there is an…
In the current density functional theory of linear and nonlinear time-dependent phenomena, the treatment of exchange and correlation beyond the level of the adiabatic local density approximation is shown to lead to the appearance of…
By propagating the many-body Schr\"odinger equation, we determine the exact time-dependent Kohn-Sham potential for a system of strongly correlated electrons which undergo field-induced tunneling. Numerous features are entirely absent from…
In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a…