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Variational algorithms for strongly correlated chemical and materials systems are one of the most promising applications of near-term quantum computers. We present an extension to the variational quantum eigensolver that approximates the…

Quantum Physics · Physics 2020-08-26 William J. Huggins , Joonho Lee , Unpil Baek , Bryan O'Gorman , K. Birgitta Whaley

Variational ab-initio methods in quantum chemistry stand out among other methods in providing direct access to the wave function. This allows in principle straightforward extraction of any other observable of interest, besides the energy,…

Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…

Chemical Physics · Physics 2026-05-07 Steven R. White

We use a variational Monte Carlo algorithm to solve the electronic structure of two-dimensional semiconductor quantum dots in external magnetic field. We present accurate many-body wave functions for the system in various magnetic field…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Ari Harju

We introduce highly local basis sets for electronic structure which are very efficient for correlation calculations near the complete basis set limit. Our approach is based on gausslets, recently introduced wavelet-like smooth orthogonal…

Chemical Physics · Physics 2019-02-20 Steven R. White , E. Miles Stoudenmire

We propose a new variational Monte Carlo (VMC) method with an energy variance extrapolation for large-scale shell-model calculations. This variational Monte Carlo is a stochastic optimization method with a projected correlated condensed…

Nuclear Theory · Physics 2012-02-14 Takahiro Mizusaki , Noritaka Shimizu

Application of diffusion Monte Carlo algorithm in three-body systems is studied. We develop a program and use it to calculate the property of various three-body systems. Regular Coulomb systems such as atoms, molecules and ions are…

Nuclear Theory · Physics 2018-04-23 Mengjiao Lyu , Zhongzhou Ren , Qihu Lin

Perhaps the simplest first-principles approach to electronic structure is to fit the charge distribution of each orbital pair and use those fits wherever they appear in the entire electron-electron (EE) interaction energy. The charge…

Chemical Physics · Physics 2015-11-10 Brett I Dunlap , Mark C Palenik

Quantum Monte Carlo (QMC) is an advanced simulation methodology for studies of manybody quantum systems. In this review, we focus on the electronic structure QMC, i.e., methods relevant for systems described by the electron-ion…

Other Condensed Matter · Physics 2010-08-16 Michal Bajdich , Lubos Mitas

We present a framework of an auxiliary field quantum Monte Carlo (QMC) method for multi-orbital Hubbard models. Our formulation can be applied to a Hamiltonian which includes terms for on-site Coulomb interaction for both intra- and…

Strongly Correlated Electrons · Physics 2009-10-30 Yukitoshi Motome , Masatoshi Imada

A novel Gaussian-Sinc mixed basis set for the calculation of the one-electron electronic structure within a uniform magnetic field in three dimensions is presented. The one-electron system is used to demonstrate the utility of this new…

Computational Physics · Physics 2014-11-12 Jonathan L. Jerke , Young Lee , C. J. Tymczak

The real-space variation quantum Monte Carlo (VMC) and diffusion quantum Monte Carlo (DMC) are used to calculate the quasiparticle energy bands and the quasiparticle effective mass of the paramagnetic and ferromagnetic two-dimensional…

Strongly Correlated Electrons · Physics 2025-11-07 S. Azadi , N. D. Drummond , A. Principi , R. V. Belosludov , M. S. Bahramy

We develop and implement a Gaussian approach to calculate partial cross-sections and asymmetry parameters for molecular photoionization. Optimal sets of complex Gaussian-type orbitals (cGTOs) are first obtained by non-linear optimization,…

Chemical Physics · Physics 2021-11-17 Abdallah Ammar , Lorenzo Ugo Ancarani , Arnaud Leclerc

A simple and stable method for computing accurate expectation values of observable with Variational Monte Carlo (VMC) or Diffusion Monte Carlo (DMC) algorithms is presented. The basic idea consists in replacing the usual ``bare'' estimator…

Chemical Physics · Physics 2009-11-10 Roland Assaraf , Michel Caffarel

Various strategies to implement efficiently QMC simulations for large chemical systems are presented. These include: i.) the introduction of an efficient algorithm to calculate the computationally expensive Slater matrices. This novel…

Performance · Computer Science 2019-05-28 Anthony Scemama , Michel Caffarel , Emmanuel Oseret , William Jalby

The study of alloys using computational methods has been a difficult task due to the usually unknown stoichiometry and local atomic ordering of the different structures experimentally. In order to combat this, first-principles methods have…

Materials Science · Physics 2021-12-08 Daniel Wines , Kayahan Saritas , Can Ataca

We present high-precision quantum computing simulations of three-body atoms (He, H$^-$) and molecules (H$_2^+$, HD$^+$), the latter being studied beyond the Born-Oppenheimer approximation. The Non-Iterative Disentangled Unitary Coupled…

Quantum Physics · Physics 2025-10-22 Mohammad Haidar , Hugo D. Nogueira , J. -Ph. Karr

A two level sampling method is applied to variational Monte Carlo (VMC) that samples the one and two body parts of the wave function separately. The method is demonstrated on a single Li_2 molecule in free space and 32 H_2 molecules in a…

Computational Physics · Physics 2016-09-08 Mark Dewing

Ab initio quantum Monte Carlo (QMC) methods are state-of-the-art electronic structure calculations based on highly parallelizable stochastic frameworks for accurate solutions of the many-body Schr{\"o}dinger equation, suitable for modern…

Chemical Physics · Physics 2026-04-07 Kousuke Nakano , Stefano Battaglia , Jürg Hutter

In electronic structure theory, variational methods offer a valuable paradigm for approximating electronic ground states. However, for historical reasons, this principle is mostly restricted to model chemistries in pre-defined fixed basis…

Quantum Physics · Physics 2025-11-17 Fabian Langkabel , Stefan Knecht , Jakob S. Kottmann