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We present a spin-dependent localized Hartree-Fock (SLHF) density-functional approach for the treatment of the inner-shell excited-state calculation of atomic systems. In this approach, the electron spin-orbitals in an electronic…

Atomic Physics · Physics 2009-11-11 Zhongyuan Zhou , Shih-I Chu

We present a novel joint time-dependent density-functional theory for the description of solute-solvent systems in time-dependent external potentials. Starting with the exact quantum-mechanical action functional for both electrons and…

Materials Science · Physics 2012-02-16 Johannes Lischner , T. A. Arias

In this paper, the performance of more than 40 popular or recently developed density functionals is assessed for the calculation of 463 vertical excitation energies against the large and accurate QuestDB benchmark set. For this purpose, the…

Chemical Physics · Physics 2022-05-19 Jiashu Liang , Xintian Feng , Diptarka Hait , Martin Head-Gordon

Modern software engineering of electronic structure codes has seen a paradigm shift from monolithic workflows towards object-based modularity. Software objectivity allows for greater flexibility in the application of electronic structure…

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…

Chemical Physics · Physics 2019-09-30 Xuelan Wen , Daniel S. Graham , Dhabih V. Chulhai , Jason D. Goodpaster

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…

Chemical Physics · Physics 2018-05-23 Per-Arno Plötz , Jörg Megow , Thomas Niehaus , Oliver Kühn

The Targeted Free Energy Perturbation (TFEP) method aims to overcome the time-consuming and computer-intensive stratification process of standard methods for estimating the free energy difference between two states. To achieve this, TFEP…

Chemical Physics · Physics 2023-02-24 Soo Jung Lee , Amr H. Mahmoud , Markus A. Lill

Transformer-based Diffusion Probabilistic Models (DPMs) have shown more potential than CNN-based DPMs, yet their extensive computational requirements hinder widespread practical applications. To reduce the computation budget of…

Computer Vision and Pattern Recognition · Computer Science 2024-11-01 Xinwang Chen , Ning Liu , Yichen Zhu , Feifei Feng , Jian Tang

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

In this study, we explore the potential of machine learning for modeling molecular electronic spectral intensities as a continuous function in a given wavelength range. Since presently available chemical space datasets provide excitation…

Chemical Physics · Physics 2022-08-02 Prakriti Kayastha , Sabyasachi Chakraborty , Raghunathan Ramakrishnan

Accurate and efficient simulation of excited state properties is an important and much aspired cornerstone in the study of adsorbate dynamics on metal surfaces. To this end, the recently proposed linear expansion \Delta Self-Consistent…

Materials Science · Physics 2013-07-23 Reinhard J. Maurer , Karsten Reuter

Accurate prediction of adiabatic $0$-$0$ excited-state energies is crucial for modeling molecular photophysical processes. Here, we benchmark computational strategies for evaluating excited-state energies and singlet-triplet gaps obtained…

Chemical Physics · Physics 2026-05-08 Amrita Bera , Atreyee Majumdar , Raghunathan Ramakrishnan

Complete computation of turbulent combustion flow involves two separate steps: mapping reaction kinetics to low-dimensional manifolds and looking-up this approximate manifold during CFD run-time to estimate the thermo-chemical state…

Machine Learning · Computer Science 2022-11-28 Amol Salunkhe , Georgios Georgalis , Abani Patra , Varun Chandola

Parameterized tight-binding models fit to first principles calculations can provide an efficient and accurate quantum mechanical method for predicting properties of molecules and solids. However, well-tested parameter sets are generally…

Materials Science · Physics 2023-04-28 Kevin F. Garrity , Kamal Choudhary

Linear response time dependent density functional theory (TDDFT), which builds upon configuration interaction singles (CIS) and TD-Hartree-Fock (TDHF), is the most widely used class of excited state quantum chemistry methods and is often…

Chemical Physics · Physics 2019-10-14 Diptarka Hait , Adam Rettig , Martin Head-Gordon

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

The electronic and magnetic properties of many strongly-correlated systems are controlled by a limited number of states, located near the Fermi level and well isolated from the rest of the spectrum. This opens a formal way for combining the…

Strongly Correlated Electrons · Physics 2010-07-15 I. V. Solovyev

We report a local, weight-dependent correlation density-functional approximation that incorporates information about both ground and excited states in the context of density-functional theory for ensembles (eDFT). This density-functional…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Emmanuel Fromager

We present a modification of the $\Delta$SCF method of calculating energies of excited states, in order to make it applicable to resonance calculations of molecules adsorbed on metal surfaces, where the molecular orbitals are highly…

Materials Science · Physics 2009-03-06 Jeppe Gavnholt , Thomas Olsen , Mads Engelund , Jakob Schiøtz