Related papers: Long-range correction for tight-binding TD-DFT
Adiabatic approximations in time-dependent density functional theory (TDDFT) will in general yield unphysical time-dependent shifts in the resonance positions of a system driven far from its ground-state. This spurious time-dependence is…
Methods based on propagation of the one-body reduced density-matrix hold much promise for the simulation of correlated many-electron dynamics far from equilibrium, but difficulties with finding good approximations for the interaction term…
Intermolecular charge-transfer is a highly important process in biology and energy-conversion applications where generated charges need to be transported over several moieties. However, its theoretical description is challenging since the…
Calculating highly accurate thermochemical properties of condensed matter via wave function-based approaches (such as e.g. Hartree-Fock or hybrid functionals) has recently attracted much interest. We here present two strategies providing…
Using time-dependent current-density functional theory, we derive analytically the dynamical exchange-correlation correction to the DC conductance of nanoscale junctions. The correction pertains to the conductance calculated in the…
We formulate a time-dependent density-matrix functional theory (TDDMFT) approach for higher-order correlation effects like biexcitons in optical processes in solids based on the reduced two-particle density-matrix formalism within the…
The Hartree-Fock exchange potential is fundamental for capturing quantum mechanical exchange effects but faces critical challenges in large-scale applications due to its nonlocal and computationally intensive nature. This study introduces a…
Ensemble density functional theory (eDFT) is an exact time-independent alternative to time-dependent DFT (TD-DFT) for the calculation of excitation energies. Despite its formal simplicity and advantages in contrast to TD-DFT (multiple…
We study the dynamics of charge-transfer insulators after photo-excitation using the three-band Emery model and a nonequilibrium extension of Hartree-Fock+EDMFT and GW+EDMFT. While the equilibrium properties are accurately reproduced by the…
We illustrate the scope of Time Dependent Density Functional Theory (TDDFT) for strongly correlated (lattice) models out of equilibrium. Using the exact many body time evolution, we reverse engineer the exact exchange correlation (xc)…
We present a new velocity-gauge real-time, time-dependent density functional tight-binding (VG-rtTDDFTB) implementation in the open-source DFTB+ software package (https://dftbplus.org) for probing electronic excitations in large, condensed…
A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…
We present a new methodology to calculate the strong light-matter coupling between photonic modes in microcavities and large molecular aggregates that consist of hundreds of molecular fragments. To this end, we combine our fragment…
The strength functions of quadrupole modes in the unstable oxygen isotopes 22O and 24O are calculated using an extended version of the time-dependent Hartree-Fock theory known as the time-dependent density-matrix theory (TDDM). It is found…
A challenge in modeling time-dependent strong-field processes such as high-harmonic generation for many-body systems, is how to effectively represent the electronic continuum. We apply Rothe's method to the time-dependent Hartree-Fock…
Hybrid density functional theory (DFT) remains intractable for large periodic systems due to the demanding computational cost of exact exchange. We apply the tensor hypercontraction (THC) (or interpolative separable density fitting)…
We formulate a time-dependent density functional theory (TDDFT) in terms of the density matrix to study ultrafast phenomena in semiconductor structures. A system of equations for the density matrix components, which is equivalent to the…
During the last two decades density functional based linear response approaches have become the de facto standard for the calculation of optical properties of small and medium-sized molecules. At the heart of these methods is the solution…
Recently, Tao and Mo proposed an accurate meta-generalized gradient approximation for the exchange-correlation energy. The exchange part is derived from the density matrix expansion, while the correlation part is obtained by improving the…
A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…