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We present a stable and systematically improvable quantum Monte Carlo (QMC) approach to calculating excited-state energies, which we implement using our fast randomized iteration method for the full configuration interaction problem…

Computational Physics · Physics 2023-10-03 Samuel M. Greene , Robert J. Webber , James E. T. Smith , Jonathan Weare , Timothy C. Berkelbach

We show that the recently developed phaseless auxiliary-field quantum Monte Carlo (AFQMC) method can be used to study excited states, providing an alternative to standard quantum chemistry methods. The phaseless AFQMC approach, whose…

Computational Physics · Physics 2013-07-09 Wirawan Purwanto , Shiwei Zhang , Henry Krakauer

We systematically investigate the calculation of excited states in quantum chemistry using auxiliary field quantum Monte Carlo (AFQMC). Symmetry allows targeting of the lowest triplet excited states in AFQMC based on restricted open-shell…

Chemical Physics · Physics 2025-09-16 Ankit Mahajan , Sandeep Sharma , Shiwei Zhang , David R. Reichman

We present developments in the calculation of reduced density matrices (RDMs) in the full configuration interaction quantum Monte Carlo (FCIQMC) method. An efficient scheme is described to allow storage of RDMs across distributed memory,…

Computational Physics · Physics 2017-07-27 N. S. Blunt , George H. Booth , Ali Alavi

Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schr\"odinger equation that scales favorably for large systems is…

Chemical Physics · Physics 2023-01-19 Mike Entwistle , Zeno Schätzle , Paolo A. Erdman , Jan Hermann , Frank Noé

We present a hybrid quantum-classical Green's function Monte Carlo (GFMC) algorithm for estimating the excited states of the nuclear shell model. The conventional GFMC method, widely used to find the ground state of a quantum many-body…

Quantum Physics · Physics 2025-08-25 Yongdan Yang , Ruyu Yang , Xiaosi Xu

Full configuration interaction quantum Monte Carlo (FCIQMC) is a stochastic approach for finding the ground state of a quantum many-body Hamiltonian. It is based on the dynamical evolution of a walker population in Hilbert space, which…

Quantum Gases · Physics 2020-11-04 Mingrui Yang , Elke Pahl , Joachim Brand

In this communication, we propose a method for obtaining isolated excited states within the Full Configuration Interaction Quantum Monte Carlo framework. This method allows for stable sampling with respect to collapse to lower energy states…

Strongly Correlated Electrons · Physics 2014-10-10 George H. Booth , Garnet Kin-Lic Chan

We introduce a family of methods for the full configuration interaction problem in quantum chemistry, based on the fast randomized iteration (FRI) framework [L.-H. Lim and J. Weare, SIAM Rev. 59, 547 (2017)]. These methods, which we term…

Chemical Physics · Physics 2023-09-25 Samuel M. Greene , Robert J. Webber , Jonathan Weare , Timothy C. Berkelbach

We extend the scope of full configuration interaction quantum Monte Carlo (FCIQMC) to be applied to coupled fermion-boson hamiltonians, alleviating the a priori truncation in boson occupation which is necessary for many other wave function…

Strongly Correlated Electrons · Physics 2022-11-09 Robert J. Anderson , Charles C. J. Scott , George H. Booth

A variational Monte Carlo method is used to generate sets of orthogonal trial functions, Psi_T(J^pi,T), for given quantum numbers in various light p-shell nuclei. These Psi_T are then used as input to Green's function Monte Carlo…

Nuclear Theory · Physics 2008-11-26 Steven C. Pieper , R. B. Wiringa , J. Carlson

Quantum Monte Carlo (QMC) is a stochastic method which has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that, within a…

Chemical Physics · Physics 2018-08-09 Anthony Scemama , Anouar Benali , Denis Jacquemin , Michel Caffarel , Pierre-François Loos

We present a discussion of recent progress in excited-state-specific quantum chemistry and quantum Monte Carlo alongside a demonstration of how a combination of methods from these two fields can offer reliably accurate excited state…

Chemical Physics · Physics 2023-02-07 Leon Otis , Eric Neuscamman

Using the homogeneous electron gas (HEG) as a model, we investigate the sources of error in the `initiator' adaptation to Full Configuration Interaction Quantum Monte Carlo (i-FCIQMC), with a view to accelerating convergence. In particular…

Computational Physics · Physics 2012-06-26 James J. Shepherd , George H. Booth , Ali Alavi

We discuss a new numerical method for the determination of excited states of a quantum system using a generalization of the Feynman-Kac formula. The method relies on introducing an ensemble of non-interacting identical systems with a…

High Energy Physics - Lattice · Physics 2008-11-26 Z. Burda , Pawel Sawicki

We provide a spin-adapted formulation of the Full Configuration Interaction Quantum Monte Carlo (FCIQMC) algorithm, based on the Graphical Unitary Group Approach (GUGA), which enables the exploitation of SU(2) symmetry within this…

Chemical Physics · Physics 2019-09-10 Werner Dobrautz , Simon Smart , Ali Alavi

We expand upon the recent semi-stochastic adaptation to full configuration interaction quantum Monte Carlo (FCIQMC). We present an alternate method for generating the deterministic space without a priori knowledge of the wave function and…

Computational Physics · Physics 2015-11-17 N. S. Blunt , Simon D. Smart , J. A. F. Kersten , J. S. Spencer , George H. Booth , Ali Alavi

Accurate ab initio calculations of 3d transition metal monoxide molecules have attracted extensive attention because of its relevance in physical and chemical science, as well as theoretical challenges in treating strong electron…

Strongly Correlated Electrons · Physics 2021-11-02 Tonghuan Jiang , Yilin Chen , Nikolay Bogdanov , Enge Wang , Ali Alavi , Ji Chen

Quantum Monte Carlo methods are first-principle approaches that approximately solve the Schr\"odinger equation stochastically. As compared to traditional quantum chemistry methods, they offer important advantages such as the ability to…

Chemical Physics · Physics 2020-02-11 Jonas Feldt , Claudia Filippi

We investigate the sign problem for full configuration interaction quantum Monte Carlo (FCIQMC), a stochastic algorithm for finding the ground state solution of the Schr\"odinger equation with substantially reduced computational cost…

Computational Physics · Physics 2014-11-05 James J. Shepherd , Gustavo E. Scuseria , James S. Spencer
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