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We propose here a single Pfaffian correlated variational ansatz, that dramatically improves the accuracy with respect to the single determinant one, while remaining at a similar computational cost. A much larger correlation energy is indeed…

Chemical Physics · Physics 2020-07-28 Claudio Genovese , Tomonori Shirakawa , Kousuke Nakano , Sandro Sorella

We present high-accuracy correlated calculations of small Si$_x$H$_y$ molecular systems both in the ground and excited states. We employ quantum Monte Carlo (QMC) together with a variety of many-body wave function approaches based on basis…

Chemical Physics · Physics 2020-10-21 Guangming Wang , Abdulgani Annaberdiyev , Lubos Mitas

Approximate natural orbitals are investigated as a way to improve a Monte Carlo configuration interaction (MCCI) calculation. We introduce a way to approximate the natural orbitals in MCCI and test these and approximate natural orbitals…

Chemical Physics · Physics 2013-04-12 J. P. Coe , M. J. Paterson

The many-body diffusion quantum Monte Carlo (DMC) method with twist-averaged boundary conditions is used to calculate the ground-state equation of state and the energetics of point defects in fcc aluminum using supercells up to 1331 atoms.…

Materials Science · Physics 2012-10-22 Randolph Q. Hood , P. R. C. Kent , Fernando A. Reboredo

Diffusion Monte Carlo (DMC) simulations for fermions are becoming the standard to provide high quality reference data in systems that are too large to be investigated via quantum chemical approaches. DMC with the fixed-node approximation…

Chemical Physics · Physics 2016-07-06 Andrea Zen , Sandro Sorella , Michael J. Gillan , Angelos Michaelides , Dario Alfè

Accurate determination of electronic properties of correlated oxides remains a significant challenge for computational theory. Traditional Hubbard-corrected density functional theory (DFT+U) frequently encounters limitations in precisely…

Materials Science · Physics 2024-03-19 Hyeondeok Shin , Kevin Gasperich , Tomas Rojas , Anh T. Ngo , Jaron T. Krogel , Anouar Benali

Quantum Monte Carlo (QMC) methods have received considerable attention over the last decades due to their great promise for providing a direct solution to the many-body Schrodinger equation in electronic systems. Thanks to their low scaling…

Chemical Physics · Physics 2013-03-28 M. A. Morales , J. McMinis , B. K. Clark , J. Kim , G. Scuseria

We propose using the wave function generated by the quantum selected configuration interaction (QSCI) method as the trial wave function in phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC). In the QSCI framework, electronic…

Full configuration interaction quantum Monte Carlo (FCIQMC) is a state-of-the-art stochastic electronic structure method, providing a methodology to compute FCI-level state energies of molecular systems within a quantum chemical basis.…

Chemical Physics · Physics 2022-04-29 Tonghuan Jiang , Wei Fang , Ali Alavi , Ji Chen

The quantum Monte Carlo (QMC) is one of the most promising many-body electronic structure approaches. It employs stochastic techniques for solving the stationary Schr\" odinger equation and for evaluation of expectation values. The key…

Other Condensed Matter · Physics 2007-12-20 Michal Bajdich

We develop a numerically exact method for the summation of irreducible Feynman diagrams for fermionic self-energy in the thermodynamic limit. The technique, based on the Diagrammatic Determinant Monte Carlo and its recent extension to…

Strongly Correlated Electrons · Physics 2019-09-11 Fedor Simkovic IV. , Evgeny Kozik

Diffusion Monte Carlo (DMC) is being recognized as a higher-accuracy, albeit more computationally expensive, alternative to Density Functional Theory (DFT) for energy predictions of catalytic systems. A major computational bottleneck in the…

Materials Science · Physics 2022-10-12 Gopal R. Iyer , Brenda M. Rubenstein

Phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) has emerged as a promising electronic structure method for correlated electronic systems. However, the quality of its predictions depends critically on the choice of trial…

Chemical Physics · Physics 2026-05-06 Don Danilov , Brad Ganoe , Leon Otis , Zhi Gong , Zixiang Lu , James Shee

Quantum Monte Carlo (QMC) techniques are used to calculate the one-body density matrix and excitation energies for the valence electrons of bulk silicon. The one-body density matrix and energies are obtained from a Slater-Jastrow wave…

Condensed Matter · Physics 2009-10-31 P. R. C. Kent , Randolph Q. Hood , M. D. Towler , R. J. Needs , G. Rajagopal

Recent technical advances in dealing with finite-size errors make quantum Monte Carlo methods quite appealing for treating extended systems in electronic structure calculations, especially when commonly-used density functional theory (DFT)…

Materials Science · Physics 2016-10-06 Kyle G. Reeves , Yi Yao , Yosuke Kanai

We provide a pedagogical introduction to the two main variants of real-space quantum Monte Carlo methods for electronic-structure calculations: variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC). Assuming no prior knowledge on…

Chemical Physics · Physics 2015-08-13 Julien Toulouse , Roland Assaraf , C. J. Umrigar

We apply the method of Monte Carlo configuration interaction (MCCI) to calculate ground-state potential energy curves for a range of small molecules and compare the results with full configuration interaction. We show that the MCCI…

Chemical Physics · Physics 2012-12-12 J. P. Coe , D. J. Taylor , M. J. Paterson

Piecewise deterministic Markov process samplers are attractive alternatives to Metropolis--Hastings algorithms. A central design question is how to incorporate partial velocity refreshment to ensure ergodicity without injecting excessive…

Probability · Mathematics 2026-02-20 Hirofumi Shiba , Kengo Kamatani

We develop a quantum Monte Carlo method to estimate the ground-state energy of a fermionic many-particle system in the configuration-interaction shell model approach. The fermionic sign problem is circumvented by using a guiding wave…

Nuclear Theory · Physics 2015-06-15 Abhishek Mukherjee , Y. Alhassid

A method is suggested to build simple multiconfigurational wave functions specified uniquely by an energy cutoff $\Lambda$. These are constructed from a model space containing determinants with energy relative to that of the most stable…

Chemical Physics · Physics 2015-06-19 Francesco A. Evangelista