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We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…

Chemical Physics · Physics 2015-06-23 Ralph Gebauer , Morrel H. Cohen , Roberto Car

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…

Chemical Physics · Physics 2016-12-04 Ralph Gebauer , Morrel H. Cohen , Roberto Car

The calculations of electronic transport coefficients and optical properties require a very dense interpolation of the electronic band structure in reciprocal space that is computationally expensive and may have issues with band crossing…

Electron microscopy is a powerful tool for studying the properties of materials down to their atomic structure. In many cases, the quantitative interpretation of images requires simulations based on atomistic structure models. These…

We present a new methodology to analyze complicated multi-physics simulations by introducing a fictitious parameter. Using the method, we study quantum mechanical aspects of an organic molecule in water. The simulation is variationally…

Chaotic Dynamics · Physics 2007-05-23 Toshiya Takami , Jun Maki , Jun-ichi Ooba , Taizo Kobayashi , Rie Nogita , Mutsumi Aoyagi

An approximate relativistic two-component Hamiltonian for use in molecular electronic structure calculations is derived in the form of a sum of fixed atom-centered kinetic and spin-orbit operators added to the non-relativistic Hamiltonian.…

Chemical Physics · Physics 2019-02-13 Dimitri N. Laikov

The quantum simulation of real molecules and materials is one of the most highly anticipated applications of quantum computing. Algorithms for simulating electronic structure using a first-quantized plane wave representation are especially…

Quantum Physics · Physics 2025-01-22 William J. Huggins , Oskar Leimkuhler , Torin F. Stetina , K. Birgitta Whaley

This chapter provides a tutorial overview of first principles methods to describe the properties of matter at the ground state or equilibrium. It begins with a brief introduction to quantum and statistical mechanics for predicting the…

Computational Engineering, Finance, and Science · Computer Science 2020-10-14 Jianzhong Wu , Mengyang Gu

The symmetry-projected Hartree--Fock ansatz for the electronic structure problem can efficiently account for static correlation in molecules, yet it is often unable to describe dynamic correlation in a balanced manner. Here, we consider a…

Strongly Correlated Electrons · Physics 2015-06-17 Carlos A. Jiménez-Hoyos , R. Rodríguez-Guzmán , Gustavo E. Scuseria

First-principles calculation of nonlinear magneto-optical effects has become an indispensable tool to reveal the geometric and topological nature of electronic states and to understand light-matter interactions. While intriguingly rich…

Materials Science · Physics 2022-02-23 Haowei Chen , Meng Ye , Nianlong Zou , Bing-lin Gu , Yong Xu , Wenhui Duan

Understanding and predicting the properties of solid-state materials from first-principles has been a great challenge for decades. Owing to the recent advances in quantum technologies, quantum computations offer a promising way to achieve…

First-principles calculations combining density functional theory and many-body perturbation theory can provide microscopic insight into the dynamics of electrons and phonons in materials. We review this theoretical and computational…

Materials Science · Physics 2016-11-23 Marco Bernardi

A method for carrying out semiclassical initial value representation calculations using first-principles molecular dynamics (FP-SC-IVR) is presented. This method can extract the full vibrational power spectrum of carbon dioxide from a…

Materials Science · Physics 2009-06-14 Michele Ceotto , Sule Atahan , Sangwoo Shim , Gianfranco Tantardini , Alán Aspuru-Guzik

Computing many-body ground state energies and resolving electronic structure calculations are fundamental problems for fields such as quantum chemistry or condensed matter. Several quantum computing algorithms that address these problems…

Quantum Physics · Physics 2023-01-12 Karen J. Morenz Korol , Kenny Choo , Antonio Mezzacapo

We introduce a novel computational approach for the investigation of complex correlated electron materials which makes it possible to evaluate interatomic forces and thereby determine atomic displacements and structural transformations…

Strongly Correlated Electrons · Physics 2014-04-24 I. Leonov , V. I. Anisimov , D. Vollhardt

We present a set of efficient techniques in first-principles electronic-structure calculations utilizing the real-space finite-difference method. These techniques greatly reduce the overhead for performing integrals that involve…

Materials Science · Physics 2009-11-10 Tomoya Ono , Kikuji Hirose

We present an efficient \textit{ab initio} method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to…

Strongly Correlated Electrons · Physics 2014-07-01 Y. X. Yao , J. Liu , C. Liu , W. C. Lu , C. Z. Wang , K. M. Ho

The recent development of multidimensional ultrafast spectroscopy techniques calls for the introduction of computational schemes that allow for the simulation of such experiments and the interpretation of the corresponding results from a…

Mesoscale and Nanoscale Physics · Physics 2023-10-30 Jannis Krumland , Michele Guerrini , Antonietta De Sio , Christoph Lienau , Caterina Cocchi

We present a method for the calculation of electronic structure of systems that contain tens of thousands of atoms. The method is based on the division of the system into mutually overlapping fragments and the representation of the…

Materials Science · Physics 2011-03-09 Nenad Vukmirović , Lin-Wang Wang

We present a method for calculating the electronic structure of correlated materials based on a truly first-principles LDA+U scheme. Recently we suggested how to calculate U from first-principles, using a method which we named constrained…

Strongly Correlated Electrons · Physics 2010-06-17 K. Karlsson , F. Aryasetiawan , O. Jepsen