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Electronic coupling matrix elements are important to the theoretical description of electron transfer processes. However, they are notoriously difficult to obtain accurately from time- dependent density functional theory (TDDFT). Here, we…

Chemical Physics · Physics 2018-12-07 Debashree Manna , Jochen Blumberger , Jan M. L. Martin , Leeor Kronik

A robust and efficient frequency dependent and non-local exchange-correlation $f_{xc}(r,r';\omega)$ is derived by imposing time-dependent density-functional theory (TDDFT) to reproduce the many-body diagrammatic expansion of the…

Materials Science · Physics 2009-11-10 A. Marini , R. Del Sole , A. Rubio

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…

Chemical Physics · Physics 2025-03-25 Chenyu Liu , Yang Xu , Peng Bao , Yangyi Lu , Jiali Gao

Site-occupation embedding theory (SOET) is an alternative formulation of density-functional theory (DFT) for model Hamiltonians where the fully-interacting Hubbard problem is mapped, in principle exactly, onto an impurity-interacting…

Strongly Correlated Electrons · Physics 2018-06-13 Bruno Senjean , Naoki Nakatani , Masahisa Tsuchiizu , Emmanuel Fromager

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…

Materials Science · Physics 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

We propose a computationally efficient approach to the nonadiabatic time-dependent density functional theory (TDDFT) which is based on a representation of the frequency-dependent exchange correlation kernel as a response of a set of damped…

Mesoscale and Nanoscale Physics · Physics 2019-12-18 Dmitry R. Gulevich , Yaroslav V. Zhumagulov , Alexei V. Vagov , Vasili Perebeinos

Theoretical studies of photochemical processes require a description of the energy surfaces of excited electronic states, especially near degeneracies, where transitions between states are most likely. Systems relevant to photochemical…

Ensemble Density Functional Theory (EDFT) is a generalization of ground-state Density Functional Theory (GS DFT), which is based on an exact formal theory of finite collections of a system's ground and excited states. EDFT in various forms…

Materials Science · Physics 2024-08-27 Remi J. Leano , Aurora Pribram-Jones , David A. Strubbe

Motivated by an experiment in which the singlet-triplet gap in triphenylene based copolymers was effectively tuned, we used time dependent density functional theory (TDDFT) to reproduce the main results. By means of conventional and…

Chemical Physics · Physics 2013-08-06 B. Kociper , T. A. Niehaus

Long-range charge transfer excited states are notoriously badly underestimated in time-dependent density functional theory (TDDFT). We resolve how {\it exact} TDDFT captures charge transfer between open-shell species: in particular the role…

Chemical Physics · Physics 2009-11-11 Neepa T. Maitra

The Quantum-Electrodynamical Time-Dependent Density Functional Theory (QED-TDDFT) equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Applications for molecules in cavities…

Quantum Physics · Physics 2022-11-30 Justin Malave , Alexander Ahrens , Daniel Pitagora , Cody Covington , Kálmán Varga

PET requires accurate, precise, and efficient scatter correction techniques. Conventional scatter estimation typically relies on tail-fitted single-scatter simulation (SSS) strategy. However, the accuracy of tail-fitted SSS is limited, for…

Nonadiabatic effects in chemical reaction at metal surfaces, due to excitation of electron-hole pairs, stand at the frontier of the studies of gas-surface reaction dynamics. However, the first principles description of electronic excitation…

Chemical Physics · Physics 2019-12-20 Yaolong Zhang , Reinhard J. Maurer , Bin Jiang

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

Inspired by the formulation of quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) by Rubio and coworkers, we propose an implementation that uses dimensionless amplitudes for describing the photonic contributions…

Materials Science · Physics 2021-08-20 Junjie Yang , Qi Ou , Zheng Pei , Hua Wang , Binbin Weng , Kieran Mullen , Yihan Shao

We present a theoretical study of the formation of self-trapped excitons (STEs) and the associated broadband emission in metal-halide perovskites Cs$_4$SnBr$_6$ and Cs$_2$AgInCl$_6$, using time-dependent density functional theory (TDDFT)…

Materials Science · Physics 2024-04-10 Yu Jin , Mariami Rusishvili , Marco Govoni , Giulia Galli

Parameter-efficient fine-tuning (PEFT) has emerged as an effective method for adapting pre-trained language models to various tasks efficiently. Recently, there has been a growing interest in transferring knowledge from one or multiple…

Computation and Language · Computer Science 2024-06-07 Zhisheng Lin , Han Fu , Chenghao Liu , Zhuo Li , Jianling Sun

Organic light emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) show increased efficiencies due to efficient upconversion of non-emissive triplet states to emissive singlets states via reverse intersystem…

Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential Vxc(r,t). An exact (i.e., nonadiabatic) extension of the…

Mesoscale and Nanoscale Physics · Physics 2015-06-25 C. A. Ullrich

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…

Mesoscale and Nanoscale Physics · Physics 2011-12-08 Miquel Huix-Rotllant , Andrei Ipatov , Angel Rubio , Mark E. Casida