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Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…

Chemical Physics · Physics 2013-07-12 Amlan K. Roy

The relativistic coupled-cluster single-double method is used to calculate the dependence of frequencies of strong $E1$-transitions in many monovalent atoms and ions on the fine-structure constant $\alpha$. These transitions are used in the…

Atomic Physics · Physics 2009-11-13 V. A. Dzuba , W. R. Johnson

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

Chemical Physics · Physics 2020-12-23 Jonathon P. Misiewicz , Justin M. Turney , Henry F. Schaefer , Alexander Yu. Sokolov

The efficient and reliable treatment of both spin-orbit coupling (SOC) and electron correlation is essential for understanding f-element chemistry. We analyze two approaches to the problem, the one-step approach where both effects are…

Chemical Physics · Physics 2022-11-09 Huanchen Zhai , Garnet Kin-Lic Chan

Evaluating multi-center molecular integrals with Cartesian Gaussian-type basis sets has been a long-standing bottleneck in electronic structure theory calculation for solids and molecules. We have developed a vector-coupling and…

Quantum Physics · Physics 2024-05-17 Hang Hu , Gilles Peslherbe , Hsu Kiang Ooi , Anguang Hu

The interaction between electronic and nuclear spins in the presence of external magnetic fields can be described by a spin Hamiltonian, with parameters obtained from first principles, electronic structure calculations. We describe an…

Materials Science · Physics 2019-04-10 Krishnendu Ghosh , He Ma , Vikram Gavini , Giulia Galli

Entanglement is the crucial ingredient of quantum many-body physics, and characterizing and quantifying entanglement in closed system dynamics of quantum simulators is an outstanding challenge in today's era of intermediate scale quantum…

Quantum Physics · Physics 2021-08-31 Christian Kokail , Rick van Bijnen , Andreas Elben , Benoît Vermersch , Peter Zoller

Relativistic dynamics of a charged particle in time-dependent electromagnetic fields has theoretical significance and a wide range of applications. It is often multi-scale and requires accurate long-term numerical simulations using…

Plasma Physics · Physics 2018-10-24 Ruili Zhang , Yulei Wang , Yang He , Jianyuan Xiao , Jian Liu , Hong Qin , Yifa Tang

Vibronic coupling has a dramatic influence over a large number of molecular processes, ranging from photo-chemistry, to spin relaxation and electronic transport. The simulation of vibronic coupling with multi-reference wavefunction methods…

Chemical Physics · Physics 2023-10-17 Lorenzo A. Mariano , Sourav Mondal , Alessandro Lunghi

A recently developed density functional method, within Hohenberg-Kohn-Sham framework, is used for faithful description of atoms, molecules in Cartesian coordinate grid, by using an LCAO-MO ansatz. Classical Coulomb potential is obtained by…

Chemical Physics · Physics 2013-07-16 Amlan K. Roy

In this paper we propose a new inexact dual decomposition algorithm for solving separable convex optimization problems. This algorithm is a combination of three techniques: dual Lagrangian decomposition, smoothing and excessive gap. The…

Optimization and Control · Mathematics 2013-02-11 Quoc Tran Dinh , Ion Necoara , Moritz Diehl

We present an accurate and efficient framework for real-space Hubbard-corrected density functional theory. In particular, we obtain expressions for the energy, atomic forces, and stress tensor suitable for real-space finite-difference…

Computational Physics · Physics 2025-10-20 Sayan Bhowmik , Andrew J. Medford , Phanish Suryanarayana

Since its inception, the ReSpect program has been evolving to provide powerful tools for simulating spectroscopic processes and exploring emerging research areas, all while incorporating relativistic effects, particularly spin-orbit…

Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…

Chemical Physics · Physics 2014-02-12 Gergely Gidofalvi , David A. Mazziotti

We study a two-grid strategy for decoupling the time-dependent Poisson-Nernst-Planck equations describing the mass concentration of ions and the electrostatic potential. The computational system is decoupled to smaller systems by using…

Numerical Analysis · Mathematics 2018-08-01 Ruigang Shen , Shi Shu , Ying Yang , Benzhuo Lu

We present a new methodology to calculate the strong light-matter coupling between photonic modes in microcavities and large molecular aggregates that consist of hundreds of molecular fragments. To this end, we combine our fragment…

Chemical Physics · Physics 2024-07-30 Richard Einsele , Luca Nils Philipp , Roland Mitrić

We present an approach for the calculation of spin density distributions for molecules that require very large active spaces for a qualitatively correct description of their electronic structure. Our approach is based on the density-matrix…

Chemical Physics · Physics 2012-06-29 Katharina Boguslawski , Konrad H. Marti , Örs Legeza , Markus Reiher

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

Quantum Physics · Physics 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

We consider different Linear Combination of Unitaries (LCU) decompositions for molecular electronic structure Hamiltonians. Using these LCU decompositions for Hamiltonian simulation on a quantum computer, the main figure of merit is the…

Quantum Physics · Physics 2023-06-13 Ignacio Loaiza , Alireza Marefat Khah , Nathan Wiebe , Artur F. Izmaylov

Reduced density matrix functional theory (RDMFT) calculations are usually implemented in a decoupled manner, where the orbital and occupation optimizations are repeated alternately. Typically, orbital updates are performed using the unitary…

Chemical Physics · Physics 2024-09-04 Yi-Fan Yao , Neil Qiang Su
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