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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…

计算物理 · 物理学 2014-10-10 George H. Booth , Deidre Cleland , Ali Alavi , David P. Tew

Full Configuration Interaction Quantum Monte Carlo (FCIQMC) has been effectively applied to very large configuration interaction (CI) problems, and was recently adapted for use as an active space solver and combined with orbital…

化学物理 · 物理学 2020-02-19 Robert J. Anderson , Toru Shiozaki , George H. Booth

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…

化学物理 · 物理学 2020-10-26 Robert J. Anderson , George H. Booth

Highly accurate results for the homogeneous electron gas (HEG) have only been achieved to date within a diffusion Monte Carlo (DMC) framework. Here, we introduce a newly developed stochastic technique, Full Configuration Interaction Quantum…

量子气体 · 物理学 2012-02-22 James J. Shepherd , George Booth , Andreas Grüneis , Ali Alavi

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…

计算物理 · 物理学 2014-11-05 James J. Shepherd , Gustavo E. Scuseria , James S. Spencer

In a recent paper, we proposed the adaptive shift method for correcting the undersampling bias of the initiator-FCIQMC. The method allows faster convergence with the number of walkers to the FCI limit than the normal initiator method,…

计算物理 · 物理学 2021-02-03 Khaldoon Ghanem , Kai Guther , Ali Alavi

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…

计算物理 · 物理学 2012-06-26 James J. Shepherd , George H. Booth , Ali Alavi

In common with many high-accuracy electronic structure methods, the initiator adaptation of full configuration interaction quantum Monte Carlo (i-FCIQMC) has difficulty treating realistic systems with large numbers of electrons. This…

We suggest an efficient method to resolve electronic cusps in electronic structure calculations by using an effective transcorrelated Hamiltonian. This effective Hamiltonian takes a simple form for plane wave bases, containing up to…

计算物理 · 物理学 2018-02-14 Hongjun Luo , Ali Alavi

The multi-reference coupled-cluster Monte Carlo (MR-CCMC) algorithm is a determinant-based quantum Monte Carlo (QMC) algorithm that is conceptually similar to Full Configuration Interaction QMC (FCIQMC). It has been shown to offer a…

强关联电子 · 物理学 2024-05-06 Zijun Zhao , Maria-Andreea Filip , Alex 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…

数值分析 · 数学 2018-06-29 Jianfeng Lu , Zhe Wang

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…

化学物理 · 物理学 2019-09-10 Werner Dobrautz , Simon Smart , Ali Alavi

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…

化学物理 · 物理学 2015-06-12 W. A. Vigor , J. S. Spencer , M. J. Bearpark , A. J. W. Thom

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…

强关联电子 · 物理学 2021-11-02 Tonghuan Jiang , Yilin Chen , Nikolay Bogdanov , Enge Wang , Ali Alavi , Ji Chen

Over the course of the past few decades, the field of computational chemistry has managed to manifest itself as a key complement to more traditional lab-oriented chemistry. This is particularly true in the wake of the recent renaissance of…

化学物理 · 物理学 2018-10-16 Janus J. Eriksen , Jürgen Gauss

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…

强关联电子 · 物理学 2022-11-09 Robert J. Anderson , Charles C. J. Scott , George H. Booth

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.…

化学物理 · 物理学 2022-04-29 Tonghuan Jiang , Wei Fang , Ali Alavi , Ji Chen

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…

计算物理 · 物理学 2015-11-17 N. S. Blunt , Simon D. Smart , J. A. F. Kersten , J. S. Spencer , George H. Booth , Ali Alavi

Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…

化学物理 · 物理学 2019-12-12 Janus J. Eriksen , Jürgen Gauss

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…

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