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The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…
We formulate a rigorous method for calculating a nonadiabatic (frequency-dependent) exchange-correlation (XC) kernel required for correct description of both equilibrium and nonequilibrium properties of strongly correlated systems within…
Standard approximations for the exchange-correlation functional have been found to give big errors for the linearity condition of fractional charges, leading to delocalization error, and the constancy condition of fractional spins, leading…
The classic density-functional theory (DFT) formalism introduced by Hohenberg, Kohn, and Sham in the mid-1960s, is based upon the idea that the complicated N-electron wavefunction can be replaced with the mathematically simpler 1-electron…
The charge-density response of extended materials is usually dominated by the collective oscillation of electrons, the plasmons. Beyond this feature, however, intriguing many-body effects are observed. They cannot be described by one of the…
We derive an exact representation of the exchange-correlation energy within density functional theory (DFT) which spawns a class of approximations leading to correct long-range asymptotic behavior. In what amounts to be the simplest…
The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…
We study linear-response time-dependent density-functional theory (DFT) based on the single-determinant range-separated hybrid (RSH) scheme, i.e. combining a long-range Hartree-Fock exchange kernel with a short-range DFT…
An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…
A complete understanding of a material requires both knowledge of the excited states as well as of the ground state. In particular, the low energy excitations are of utmost importance while studying the electronic, magnetic, dynamical, and…
We present a detailed analysis of several time-dependent DFT (TD-DFT) methods, including conventional hybrid functionals and two types of non-empirically tuned range-separated functionals, for predicting a diverse set of electronic…
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…
A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…
Electronic response properties of high-energy density (HED) systems influence planetary structure, drive evolution of fusion targets, and underpin diagnostics in laboratory astrophysics. Real-time time-dependent density functional theory…
Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…
The interaction between excited states of a closed-shell chromophore and a nearby free radical species gives rise to spin-coupled doublet states, namely singdoublet and tripdoublet, as well as a quartet state. This coupling facilitates…
Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…
Density functional theory (DFT) and linear-response time-dependent density functional theory (LR-TDDFT) rely on an exchange-correlation (xc) approximation that provides not only energy but also its functional derivatives that enter the…
Time-dependent density-functional theory (TDDFT) is a powerful tool to study the non-equilibrium dynamics of inhomogeneous interacting many-body systems. Here we show that the simple adiabatic local-spin-density approximation for the…
Time dependent quantum systems are the subject of intense inquiry, in mathematics, science, and engineering, particularly at the atomic and molecular levels. In 1984, Runge and Gross introduced time dependent density functional theory…