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Standard approximations for the exchange-correlation (XC) functional in Kohn-Sham density functional theory (KS-DFT) typically lead to unacceptably large errors when applied to strongly-correlated electronic systems. Partition-DFT (PDFT) is…

Chemical Physics · Physics 2023-09-12 Yi Shi , Yuming Shi , Adam Wasserman

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…

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

Fragmentation methods applied to multireference wave functions constitute a road towards the application of highly accurate ab initio wave function calculations to large molecules and solids. However, it is important for reproducibility and…

Chemical Physics · Physics 2020-07-23 Matthew R. Hermes , Laura Gagliardi

Multicomponent methods seek to treat select nuclei, typically protons, fully quantum mechanically and equivalent to the electrons of a chemical system. In such methods, it is well known that due to the neglect of electron-proton…

Chemical Physics · Physics 2020-12-21 O. Jonathan Fajen , Kurt R. Brorsen

We cure the lack of spin torque in semilocal exchange-correlation (XC) functionals by treating XC effects in the framework of spin-current-density-functional theory (SCDFT), and present the implementation of the first kind of this novel…

Materials Science · Physics 2025-01-09 Marie-Therese Huebsch , Fabien Tran , Martijn Marsman

The exact interaction energy of a many-electron system is determined by the electron pair density, which is not well-approximated in standard Kohn-Sham density functional models. Here we study the (complicated but well-defined) exact…

Chemical Physics · Physics 2015-08-07 Huajie Chen , Gero Friesecke

Accurately modeling photochemical reactions is difficult due to the presence of conical intersections and locally avoided crossings as well as the inherently multiconfigurational character of excited states. As such, one needs a multi-state…

Chemical Physics · Physics 2024-04-26 Matthew R. Hennefarth , Matthew R. Hermes , Donald G. Truhlar , Laura Gagliardi

As a universal quantum mechanical approach to the dynamical many-body problem, the time-dependent density functional theory (TDDFT) might be inadequate to describe crucial observables that rely on two-body evolution behavior, like the…

Computational Physics · Physics 2025-11-17 Jiong-Hang Liang , Yunfeng Xiong

Multiconfiguration pair-density functional theory (MC-PFDT) has previously been applied successfully to carry out ground-state and excited-state calculations. However, because it includes no interaction between electronic states, MC-PDFT…

We present the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method to simulate multielectron dynamics in ultrafast intense laser fields from the first principles. While based on multiconfiguration expansion, it…

Atomic Physics · Physics 2018-04-24 Takeshi Sato , Yuki Orimo , Takuma Teramura , Oyunbileg Tugs , Kenichi L. Ishikawa

The alternative separation of exchange and correlation energies proposed by Toulouse et al. [Theor. Chem. Acc. 114, 305 (2005)] is explored in the context of multi-configuration range-separated density-functional theory. The new…

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

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

We use voxel deep neural networks to predict energy densities and functional derivatives of electron kinetic energies for the Thomas-Fermi model and Kohn-Sham density functional theory calculations. We show that the ground-state electron…

Mesoscale and Nanoscale Physics · Physics 2022-01-24 Kevin Ryczko , Sebastian J. Wetzel , Roger G. Melko , Isaac Tamblyn

The classical map hypernetted-chain (CHNC) method for interacting electrons uses a kinetic energy functional in the form of a classical-fluid temperature. Here we show that the CHNC generated two-body densities and pair-distribution…

Statistical Mechanics · Physics 2019-11-11 M. W. C. Dharma-wardana

Aspects of Density Functional Resonance Theory (DFRT) [Phys. Rev. Lett. \textbf{107}, 163002 (2011)], a recently developed complex-scaled version of ground-state Density Functional Theory (DFT), are studied in detail. The asymptotic…

Quantum Physics · Physics 2015-06-04 Daniel L. Whitenack , Adam Wasserman

We have developed multi-dimensional constrained covariant density functional theories (MDC-CDFT) for finite nuclei in which the shape degrees of freedom \beta_{\lambda\mu} with even \mu, e.g., \beta_{20}, \beta_{22}, \beta_{30}, \beta_{32},…

Nuclear Theory · Physics 2014-10-23 Bing-Nan Lu , Jie Zhao , En-Guang Zhao , Shan-Gui Zhou

In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…

Materials Science · Physics 2010-04-23 Gregory C. Dente

We present a detailed comparison of the S0, S1 (n -> \pi*) and S2 (\pi -> \pi*) potential energy surfaces (PESs) of the prototypical molecular switch azobenzene as obtained by Delta-self-consistent-field (Delta-SCF) Density-Functional…

Chemical Physics · Physics 2012-02-22 Reinhard J. Maurer , Karsten Reuter