相关论文: Excited state diabatization on the cheap using DFT…

Diabatic states and the couplings between them are important for quantifying, elucidating, and predicting the rates and mechanisms of many chemical and biochemical processes. Here, we propose and investigate approaches to accurately compute…

Charge transfer (CT) processes that are electronically non-adiabatic are ubiquitous in chemistry, biology, and materials science, but their theoretical description requires diabatic states or adiabatic excited states. For complex systems,…

We introduce a novel methodology for simulating the excited-state dynamics of extensive molecular aggregates in the framework of the long-range corrected time-dependent density-functional tight-binding fragment molecular orbital method…

Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…

We propose a new block localized excitation (BLE) method to directly construct diabatic excited states without the need to first compute the adiabatic states. The new method is capable to keep any electrons, spins, and excitations localized…

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

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…

Time-dependent density functional theory (TD-DFT) and correlated ab initio methods have been applied to the electronically excited states of vitamin B12 (cyanocobalamin or CNCbl). Different experimental techniques have been used to probe…

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,…

We investigate a diabatization procedure that localizes charges (in real space) and localizes spins (in spin space) for open-shell systems that exhibit charge transfer in the presence of spin-orbit coupling. The procedure is applied to a…

Charge-transfer excited states are highly relevant for applications in molecular electronics. However, the accurate calculation of these states in large systems is challenging since wave function methods are prohibitively expensive,…

Almost all time-dependent density-functional theory (TDDFT) calculations of excited states make use of the adiabatic approximation, which implies a frequency-independent exchange-correlation kernel that limits applications to…

Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…

Density functional theory (DFT) has greatly expanded our ability to affordably compute and understand electronic ground states, by replacing intractable {\em ab initio} calculations by models based on paradigmatic physics from high- and…

We develop and test a method that integrates many-electron weak-field asymptotic theory (ME-WFAT) [Phys. Rev. A 89, 013421 (2014)] in the integral representation (IR) into the density functional theory (DFT) framework. In particular, we…

We propose a new method of calculating electronically excited states that combines a density functional theory (DFT) based ground state calculation with a linear response treatment that employs approximations used in the time-dependent…

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…

The performance of time-independent, orbital optimized calculations of excited states is assessed with respect to charge transfer excitations in organic molecules in comparison to the linear-response time-dependent density functional theory…

We present a quantum embedding method that allows for the calculation of local excited states embedded in a Kohn-Sham density functional theory (DFT) environment. Projection-based quantum embedding methodologies provide a rigorous framework…

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…