Related papers: Long-range Corrected Fragment Molecular Orbital De…
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…
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…
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…
We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): Firstly, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state…
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…
Routine investigations of plasmonic phenomena at the quantum level present a formidable computational challenge due to the large system sizes and ultrafast timescales involved. This Feature Article highlights the use of density functional…
In this work we propose a chemically-informed data-driven approach to benchmark the approximate density-functional tight-binding (DFTB) excited state (ES) methods that are currently available within the DFTB+ suite. By taking advantage of…
A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…
Spectral density functions are central to the simulation of complex many body systems. Their determination requires to make approximations not only to the dynamics but also to the underlying electronic structure theory. Here, blending…
We present an extension of the shadow extended Lagrangian Born-Oppenheimer molecular dynamics (XL-BOMD) method to excited state molecular dynamics (ESMD) in the context of \DeltaSCF Kohn-Sham density functional theory, with demonstrations…
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…
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…
Rydberg excited states of molecules pose a challenge for electronic structure calculations because of their highly diffuse electron distribution. Even large and elaborate atomic basis sets tend to underrepresent the long-range tail, overly…
A derivation of non-adiabatic coupling vectors for the density functional based tight binding method (DFTB) between ground and excited states is presented. The analytical result is valid both for semi-local and long-range corrected DFTB and…
The software package DIALECT is introduced, which provides the capability of calculating excited-state properties and nonadiabatic dynamics of large molecular systems and can be applied to simulate energy and charge-transfer processes in…
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…
The Frenkel exciton Hamiltonian is at the heart of many simulations of excitation energy transfer in molecular aggregates. It separates the aggregate into Coulomb-coupled monomers. Here it is shown that the respective parameters, i.e.…
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,…
This article is a pedagogical introduction to density-functional tight-binding (DFTB) method. We derive it from the density-functional theory, give the details behind the tight-binding formalism, and give practical recipes for…
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,…