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In this work, we introduce three algorithmic improvements to reduce the cost and improve the scaling of orbital space variational Monte Carlo (VMC). First, we show that by appropriately screening the one- and two-electron integrals of the…

Chemical Physics · Physics 2018-07-30 Iliya Sabzevari , Sandeep Sharma

Valence-bond-based wavefunctions, such as the spin-coupled generalized valence bond (SCGVB) ansatz, provide compact and chemically interpretable descriptions of strong correlation. However, their non-orthogonal determinant structure poses a…

Quantum Physics · Physics 2026-04-20 Bruna Gabrielly

Variational quantum algorithms (VQAs) provide a promising approach to achieving quantum advantage for practical problems on near-term noisy intermediate-scale quantum (NISQ) devices. Thus far, most studies on VQAs have focused on…

Quantum Physics · Physics 2023-10-06 Yutaro Enomoto , Keitaro Anai , Kenta Udagawa , Shuntaro Takeda

We develop analytical gradients of ground- and excited-state energies with respect to system parameters including the nuclear coordinates for the hybrid quantum/classical multistate contracted variational quantum eigensolver (MC-VQE)…

Quantum Physics · Physics 2021-10-12 Robert M. Parrish , Gian-Luca R. Anselmetti , Christian Gogolin

The key feature of nonlocal kinetic energy functionals is their ability to reduce to the Thomas-Fermi functional in the regions of high density and to the von Weizs\"acker functional in the region of low density/high density gradient. This…

Materials Science · Physics 2021-03-31 Xuecheng Shao , Wenhui Mi , Michele Pavanello

We investigate fundamental properties of meta-generalized-gradient approximations (meta-GGAs) to the exchange-correlation energy functional, which have an implicit density dependence via the Kohn-Sham kinetic-energy density. To this…

Chemical Physics · Physics 2014-12-10 F. G. Eich , Maria Hellgren

We introduce a non-parametric density estimator deemed Radial Voronoi Density Estimator (RVDE). RVDE is grounded in the geometry of Voronoi tessellations and as such benefits from local geometric adaptiveness and broad convergence…

A global hybrid extension of variational two-electron reduced-density matrix (v2RDM)-driven multiconfiguration pair-density functional theory (MCPDFT) is developed. Using a linear decomposition of the electron-electron repulsion term, a…

Chemical Physics · Physics 2019-11-27 Mohammad Mostafanejad , Marcus Dante Liebenthal , A. Eugene DePrince

Smooth, highly accurate analytical representations of Fermi-Dirac (FD) integral combinations important in free-energy density functional calculations are presented. Specific forms include those that occur in the local density approximation…

Computational Physics · Physics 2015-04-21 Valentin V. Karasiev , Debajit Chakraborty , S. B. Trickey

We evaluate an adaptive gaussian quadrature integration scheme that will be suitable for the numerical evaluation of generalized redistribution in frequency functions. The latter are indispensable ingredients for "full non-LTE" radiation…

Instrumentation and Methods for Astrophysics · Physics 2020-01-29 F. Paletou , C. Peymirat , E. Anterrieu , T. Böhm

We study the vibrational spectrum of the protonated water dimer, by means of a divide-and-conquer semiclassical initial value representation of the quantum propagator, as a first step in the study of larger protonated water clusters. We use…

Chemical Physics · Physics 2019-09-23 Gianluca Bertaina , Giovanni Di Liberto , Michele Ceotto

A new and automated method is presented for the analysis of high-resolution absorption spectra. Three established numerical methods are unified into one "artificial intelligence" process: a genetic algorithm (GVPFIT); non-linear…

Instrumentation and Methods for Astrophysics · Physics 2017-02-01 Matthew B. Bainbridge , John K. Webb

The package "fhi96md" is an efficient code to perform density-functional theory total-energy calculations for materials ranging from insulators to transition metals. The package employs first-principles pseudopotentials, and a plane-wave…

Condensed Matter · Physics 2009-10-30 Michel Bockstedte , Alexander Kley , Joerg Neugebauer , Matthias Scheffler

A real-space formalism for density-functional perturbation theory (DFPT) is derived and applied for the computation of harmonic vibrational properties in molecules and solids. The practical implementation using numeric atom-centered…

Materials Science · Physics 2017-03-08 Honghui Shang , Christian Carbogno , Patrick Rinke , Matthias Scheffler

The past few years has brought renewed focus on the physics behind the class of materials characterized by long-range interactions and wide regions of low electron density, sparse matter. There is now much work on developing the appropriate…

Materials Science · Physics 2015-05-19 Elisa Londero , Elsebeth Schroder

Variational quantum eigensolver (VQE) is a hybrid quantum-classical algorithm designed for noisy intermediate-scale quantum (NISQ) computers. It is promising for quantum chemical calculations (QCC) because it can calculate the ground-state…

The Variational Quantum Eigensolver (VQE) is a promising algorithm for quantum computing applications in chemistry and materials science, particularly in addressing the limitations of classical methods for complex systems. This study…

Quantum Physics · Physics 2025-02-25 Nia Pollard , Kamal Choudhary

The theoretical description of sparse matter attracts much interest, in particular for those ground-state properties that can be described by density functional theory (DFT). One proposed approach, the van der Waals density functional…

Reporting extensions of a recently developed approach to density functional theory with correct long-range be-havior (Phys. Rev. Lett. 94, 043002 (2005)). The central quantities are a splitting functional gamma[n] and a complementary…

Materials Science · Physics 2017-09-13 Ester Livshits , Roi Baer

Variational quantum algorithms (VQAs) are hybrid quantum-classical approaches used for tackling a wide range of problems on noisy intermediate-scale quantum (NISQ) devices. Testing these algorithms on relevant hardware is crucial to…

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