Related papers: Efficiently computing excitations of complex syste…
We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…
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 primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…
A top-level designed forecasting system for predicting computational times of density-functional theory (DFT)/time-dependent density-functional theory (TDDFT) calculations is presented. The computational time is assumed as the intrinsic…
The accurate treatment of electron correlation in extended molecular systems remains computationally challenging using classical electronic structure methods. Hybrid quantum-classical algorithms offer a potential route to overcome these…
We introduce the concept of embedding quantum simulators, a paradigm allowing the efficient quantum computation of a class of bipartite and multipartite entanglement monotones. It consists in the suitable encoding of a simulated quantum…
We present an efficient ab initio dynamical mean-field theory (DMFT) implementation for quantitative simulations in solids. Our DMFT scheme employs ab initio Hamiltonians defined for impurities comprising the full unit cell or a supercell…
The ground state electron density -- obtainable using Kohn-Sham Density Functional Theory (KS-DFT) simulations -- contains a wealth of material information, making its prediction via machine learning (ML) models attractive. However, the…
The real-time electronic dynamics on material surfaces is critically important to a variety of applications. However, their simulations have remained challenging for conventional methods such as the time-dependent density-functional theory…
We have recently developed a method based on relativistic time-dependent density functional theory (TD-DFT) that allows the calculation of electronic spectra in solution (Creutzberg, Hedeg{\aa}rd, J. Chem. Theory Comput.18, 2022, 3671).…
We present an efficient and systematically convergent approach to all-electron real-time time-dependent density functional theory (TDDFT) calculations using a mixed basis, termed as enriched finite element (EFE) basis. The EFE basis…
We present a novel multi-scale embedding scheme that links conventional QM/MM embedding and bootstrap embedding (BE) to allow simulations of large chemical systems on limited quantum devices. We also propose a mixed-basis BE scheme that…
The projection-based quantum embedding method is applied to electronically excited states of valence, Rydberg, and charge-transfer character, valence- and core-ionized states, as well as bound and temporary radical anions. We embed…
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,…
Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…
Time-dependent density functional theory (TDDFT) is presently enjoying enormous popularity in quantum chemistry, as a useful tool for extracting electronic excited state energies. This article explains what TDDFT is, and how it differs from…
Ensemble density functional theory (EDFT) is a promising alternative to time-dependent density functional theory for computing electronic excitation energies. Using coordinate scaling, we prove several fundamental exact conditions in EDFT…
The simulation of strongly correlated electron systems remains a formidable challenge. Certain experimentally relevant dynamical response functions are especially difficult to calculate, due to issues of finite-size effects and the ill…
In principle, we should not need the time-dependent extension of density-functional theory (TDDFT) for excitations, and in particular not for Molecular Dynamics (MD) studies: the theorem by Hohenberg and Kohn teaches us that for any…
We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…