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We identify the dominant computational cost within the recently introduced stochastic and internally contracted FCIQMC-NEVPT2 method for large active space sizes. This arises from the contribution to the four-body intermediates arising from…

Chemical Physics · Physics 2020-10-05 James J. Halson , Robert J. Anderson , George H. Booth

By performing a stochastic dynamic in a space of Slater determinants, the Full Configuration Interaction Quantum Monte Carlo (FCIQMC) method has been able to obtain energies which are essentially free from systematic error to the basis set…

Computational Physics · Physics 2014-10-10 George H. Booth , Deidre Cleland , Ali Alavi , David P. Tew

The Full Configuration Interaction Quantum Monte Carlo (FCIQMC) method has proved able to provide near-exact solutions to the electronic Schr\"odinger equation within a finite orbital basis set, without relying on an expansion about a…

Computational Physics · Physics 2016-08-24 Jennifer Kersten , George H. Booth , 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

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

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

There has been recent literature discussion on the origin and severity of the `sign problem' in full configuration interaction quantum Monte Carlo (FCIQMC) and its `initiator' adaptation (i-FCIQMC), methods of interest and potential because…

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

We show that Full Configuration Interaction Quantum Monte Carlo (FCIQMC) is a Markov Chain in its present form. We construct the Markov matrix of FCIQMC for a two determinant system and hence compute the stationary distribution. These…

Chemical Physics · Physics 2015-06-12 W. A. Vigor , J. S. Spencer , M. J. Bearpark , A. J. W. Thom

In this paper, we propose a general analysis framework for inexact power iteration, which can be used to efficiently solve high dimensional eigenvalue problems arising from quantum many-body problems. Under the proposed framework, we…

Numerical Analysis · Mathematics 2018-06-29 Jianfeng Lu , Zhe Wang

An adaptation of the full configuration interaction quantum Monte Carlo (FCIQMC) method is presented, for correlated electron problems containing heavy elements and the presence of significant relativistic effects. The modified algorithm…

Chemical Physics · Physics 2020-10-26 Robert J. Anderson , George H. Booth

We present an approach to combining selected configuration interaction (SCI) and initiator full configuration interaction quantum Monte Carlo (i-FCIQMC). In the current i-FCIQMC scheme, the space of initiators is chosen dynamically by a…

Chemical Physics · Physics 2019-11-15 Nick S. Blunt

The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wave functions in large active spaces. We present a…

Chemical Physics · Physics 2020-01-08 Ankit Mahajan , Nick S. Blunt , Iliya Sabzevari , Sandeep Sharma

The convergence of full configuration interaction quantum Monte Carlo (FCIQMC) is accelerated using a quasi-Newton propagation (QN) which can also be applied to coupled cluster Monte Carlo (CCMC). The computational scaling of this optimised…

Chemical Physics · Physics 2020-06-11 Verena A. Neufeld , Alex J. W. Thom

Model space quantum Monte Carlo (MSQMC) is an extension of full configuration interaction QMC (FCIQMC) that allows us to calculate quasi-degenerate and excited electronic states by sampling the effective Hamiltonian in the model space. We…

Chemical Physics · Physics 2017-12-29 Seiichiro L. Ten-no

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

The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…

Chemical Physics · Physics 2015-10-14 Robert E. Thomas , Qiming Sun , Ali Alavi , George H. Booth

For many decades, quantum chemical method development has been dominated by algorithms which involve increasingly complex series of tensor contractions over one-electron orbital spaces. Procedures for their derivation and implementation…

Computational Physics · Physics 2014-10-10 George H. Booth , Simon D. Smart , Ali Alavi

We report internally contracted relativistic multireference configuration interaction (ic-MRCI), complete active space second-order perturbation (CASPT2), and strongly contracted n-electron valence state perturbation theory (NEVPT2) on the…

Chemical Physics · Physics 2015-12-31 Toru Shiozaki , Wataru Mizukami

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
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