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Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical ab initio method for studying solids under photoexcitation, we develop a momentum-resolved real-time time…

Materials Science · Physics 2018-10-17 Chao Lian , Shi-Qi Hu , Meng-Xue Guan , Sheng Meng

We revisit the three-body problem in quantum mechanics in two and three dimensions, generating both exact eigenvalues and eigenvectors of the Hamiltonian and a series of approximate solutions as calculated with a variety of different…

Given the time-evolution of an electron charge density, the local potential in Kohn-Sham time-dependent density functional theory (KS-TDDFT) can be modeled as a sum of instantaneous and dynamic contributions by assuming a certain form of…

Computational Physics · Physics 2016-11-09 R. J. Magyar

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…

Strongly Correlated Electrons · Physics 2015-05-27 J. L. Alonso , Alberto Castro , Pablo Echenique , Angel Rubio

We develop numerical methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta…

Materials Science · Physics 2016-01-07 Shunsuke A. Sato , Yasutaka Taniguchi , Yasushi Shinohara , Kazuhiro Yabana

Based on the quantum trajectory approach, we extend the Born-Oppenheimer (BO) approximation from closed quantum system to open quantum system, where the open quantum system is described by a master equation in Lindblad form. The BO…

Quantum Physics · Physics 2010-05-25 X. L. Huang , S. L. Wu , L. C. Wang , X. X. Yi

Real-time time-dependent density functional theory (RT-TDDFT) is known to be hindered by the very small time step (attosecond or smaller) needed in the numerical simulation due to the fast oscillation of electron wavefunctions, which…

Computational Physics · Physics 2018-10-25 Weile Jia , Dong An , Lin-Wang Wang , Lin Lin

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

Real-time, time-dependent density functional theory (RT-TDDFT) has gained popularity as a first-principles approach to study a variety of excited-state phenomena such as optical excitations and electronic stopping. Within RT-TDDFT…

Materials Science · Physics 2019-07-23 Dillon C. Yost , Yi Yao , Yosuke Kanai

We benchmark a set of quantum-chemistry methods, including multitrajectory Ehrenfest, fewest-switches surface-hopping, and multiconfigurational-Ehrenfest dynamics, against exact quantum-many-body techniques by studying real-time dynamics in…

We show that following the standard mantra of quantum chemistry and diagonalizing the Born-Oppenheimer (BO) Hamiltonian $\hat H_{\rm BO}(\bm R)$ is not the optimal means to construct potential energy surfaces. A better approach is to…

It was recently shown [G. Albareda, et al., Phys. Rev. Lett. 113, 083003 (2014)] that within the conditional decomposition approach to the coupled electron-nuclear dynamics, the electron-nuclear wave function can be exactly decomposed into…

Chemical Physics · Physics 2018-06-13 Guillermo Albareda , Ali Abedi , Ivano Tavernelli , Angel Rubio

The energy density functional (EDF) method is currently the only microscopic theoretical approach able to tackle the entire nuclear chart. Nevertheless, it suffers from limitations resulting from its empirical character and deteriorating…

Nuclear Theory · Physics 2024-04-04 Kilian Fraboulet , Jean-Paul Ebran

Orbital-free density functional theory (OFDFT) offers a challenging way of electronic-structure calculations scaled as $\mathcal{O}(N)$ computation for system size $N$. We here develop a scheme of the OFDFT calculations based on the…

Computational Physics · Physics 2021-09-06 Fumihiro Imoto , Masatoshi Imada , Atsushi Oshiyama

Describing the dynamics of nuclei in molecules requires a potential energy surface, which is traditionally provided by the Born-Oppenheimer or adiabatic approximation. However, we also need to assign masses to the nuclei. There, the…

We present an efficient quantum algorithm for beyond-Born-Oppenheimer molecular energy computations. Our approach combines the quantum full configuration interaction method with the nuclear orbital plus molecular orbital (NOMO) method. We…

Quantum Physics · Physics 2016-02-24 Libor Veis , Jakub Višňák , Hiroaki Nishizawa , Hiromi Nakai , Jiří Pittner

A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…

Chemical Physics · Physics 2020-11-06 Sudip Sasmal , Oriol Vendrell

A generalized approach of the Born-Oppenheimer approximation is developed to analytically deal with the influence exercised by the spatial motion of atom's mass-center on a two-level atom in an optical ring cavity with a quantized…

High Energy Physics - Theory · Physics 2007-05-23 Chang-Pu Sun

Nuclear quantum effects are important in a variety of chemical and biological processes. The constrained nuclear-electronic orbital density functional theory (cNEO-DFT) has been developed to include nuclear quantum effects in energy…

Chemical Physics · Physics 2021-09-20 Xi Xu , Yang Yang

We develop a phase-space electronic structure theory of molecules in magnetic fields. For a system of electrons in a magnetic field with vector potential $\bf{A}(\hat{\bf{r}})$, the usual Born-Oppenheimer Hamiltonian is the sum of the…

Chemical Physics · Physics 2024-11-25 Mansi Bhati , Zhen Tao , Xuezhi Bian , Jonathan Rawlinson , Robert Littlejohn , Joseph E. Subotnik
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