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Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…

Chemical Physics · Physics 2022-10-06 Karthik Gururangan , J. Emiliano Deustua , Jun Shen , Piotr Piecuch

In this paper we present a computational procedure that utilizes real-space grids to obtain high precision approximations of electrostatically confined few-electron states such as those that arise in gated semiconductor quantum dots. We use…

Mesoscale and Nanoscale Physics · Physics 2023-01-27 Christopher R. Anderson , Mark F. Gyure , Sam Quinn , Andrew Pan , Richard S. Ross , Andrey A. Kiselev

The recent many-body expanded full configuration interaction (MBE-FCI) method is reviewed by critically assessing its advantages and drawbacks in the context of contemporary near-exact electronic structure theory. Besides providing a…

Chemical Physics · Physics 2021-03-02 Janus J. Eriksen , Jürgen Gauss

The accurate description of electron correlation is a central challenge in computational chemistry, with selected configuration interaction (SCI) emerging as a powerful tool to approach the full CI limit. While recent machine learning (ML)…

Chemical Physics · Physics 2026-05-12 Wan Nie , Songwei Liu , Yingying Yu , Zhiwen Wang , and Jun Yang

We extend the recently proposed heat-bath configuration interaction (HCI) method [Holmes, Tubman, Umrigar, J. Chem. Theory Comput. 12, 3674 (2016)], by introducing a semistochastic algorithm for performing multireference Epstein-Nesbet…

Chemical Physics · Physics 2017-03-20 Sandeep Sharma , Adam Holmes , Guillaume Jeanmairet , Ali Alavi , C. J. Umrigar

The recently proposed many-body expanded full configuration interaction (MBE-FCI) method is extended to excited states and static first-order properties different from total, ground state correlation energies. Results are presented for…

Chemical Physics · Physics 2020-10-20 Janus J. Eriksen , Jürgen Gauss

Recent advances in selected CI, including the adaptive sampling configuration interaction (ASCI) algorithm and its heat bath extension, have made the ASCI approach competitive with the most accurate techniques available, and hence an…

Asymptotics-based configuration-interaction (CI) methods [G. Friesecke and B. D. Goddard, Multiscale Model. Simul. 7, 1876 (2009)] are a class of CI methods for atoms which reproduce, at fixed finite subspace dimension, the exact…

Quantum Physics · Physics 2012-04-06 Christian Mendl , Gero Friesecke

We present a new approach to calculate excited states with the full configuration interaction quantum Monte Carlo (FCIQMC) method. The approach uses a Gram-Schmidt procedure, instantaneously applied to the stochastically evolving…

Computational Physics · Physics 2015-10-28 N. S. Blunt , Simon D. Smart , George H. Booth , Ali Alavi

We propose the use of preconditioning in FCIQMC which, in combination with perturbative estimators, greatly increases the efficiency of the algorithm. The use of preconditioning allows a time step close to unity to be used (without…

Chemical Physics · Physics 2019-05-17 Nick S. Blunt , Alex J. W. Thom , Charles J. C. Scott

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 propose the regularized compressed double factorization (RC-DF) method to classically compute compressed representations of molecular Hamiltonians that enable efficient simulation with noisy intermediate scale (NISQ) and error corrected…

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 identify and rectify a crucial source of bias in the initiator FCIQMC algorithm. Non-initiator determinants (i.e. determinants whose population is below the initiator threshold) are subject to a systematic {\em undersampling} bias, which…

Computational Physics · Physics 2019-12-13 Khaldoon Ghanem , Alexander Y. Lozovoi , Ali Alavi

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…

Quantum Gases · Physics 2012-02-22 James J. Shepherd , George Booth , Andreas Grüneis , Ali Alavi

Finite-rate-of-innovation (FRI) signals are ubiquitous in applications such as radar, ultrasound, and time of flight imaging. Due to their finite degrees of freedom, FRI signals can be sampled at sub-Nyquist rates using appropriate sampling…

Signal Processing · Electrical Eng. & Systems 2021-07-02 Satish Mulleti , Haiyang Zhang , Yonina C. Eldar

Frequency response functions (FRFs) are important for assessing the behavior of stochastic linear dynamic systems. For large systems, their evaluations are time-consuming even for a single simulation. In such cases, uncertainty…

Computation · Statistics 2017-03-23 V. Yaghoubi , S. Marelli , B. Sudret , T. Abrahamsson

The efficiency of the recently proposed iCIPT2 [iterative configuration interaction (iCI) with selection and second-order perturbation theory (PT2); J. Chem. Theory Comput. 16, 2296 (2020)] for strongly correlated electrons is further…

Chemical Physics · Physics 2020-11-19 Ning Zhang , Wenjian Liu , Mark R. Hoffmann

In this work we propose a novel approach to solve the Schr\"{o}dinger equation which combines projection onto the ground state with a path-filtering truncation scheme. The resulting projector configuration interaction (PCI) approach…

Chemical Physics · Physics 2016-06-29 Tianyuan Zhang , Francesco A. Evangelista

In the present letter, it is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual…

Chemical Physics · Physics 2017-09-15 Janus J. Eriksen , Filippo Lipparini , Jürgen Gauss