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An iterative configuration interaction (iCI)-based multiconfigurational self-consistent field (SCF) theory, iCISCF, is proposed to handle systems that require large complete active spaces (CAS). The success of iCISCF stems from three…

Chemical Physics · Physics 2021-06-21 Yang Guo , Ning Zhang , Yibo Lei , Wenjian Liu

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,…

Computational Physics · Physics 2021-02-03 Khaldoon Ghanem , Kai Guther , Ali Alavi

Microsimulation models (MSMs) are used to predict population-level effects of health care policies by simulating individual-level outcomes. Simulated outcomes are governed by unknown parameters that are chosen so that the model accurately…

Methodology · Statistics 2018-08-14 Carolyn Rutter , Jonathan Ozik , Maria DeYoreo , Nicholson Collier

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

Multi-fidelity Bayesian optimization (MFBO) accelerates the search for the global optimum of black-box functions by integrating inexpensive, low-fidelity approximations. The central task of an MFBO policy is to balance the cost-efficiency…

Machine Learning · Computer Science 2026-02-03 Md Abir Hossen , Mohammad Ali Javidian , Vignesh Narayanan , Jason M. O'Kane , Pooyan Jamshidi

Multi fidelity Bayesian optimization (MFBO) leverages experimental and or computational data of varying quality and resource cost to optimize towards desired maxima cost effectively. This approach is particularly attractive for chemical…

Machine Learning · Computer Science 2024-09-12 Edmund Judge , Mohammed Azzouzi , Austin M. Mroz , Antonio del Rio Chanona , Kim E. Jelfs

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

Selected configuration interaction (sCI) methods including second-order perturbative corrections provide near full CI (FCI) quality energies with only a small fraction of the determinants of the FCI space. Here, we introduce both a…

Chemical Physics · Physics 2018-08-09 Yann Garniron , Anthony Scemama , Emmanuel Giner , Michel Caffarel , Pierre-François Loos

Recent advances in both theoretical and computational methods have enabled large-scale, precision calculations of the properties of atomic nuclei. With the growing complexity of modern nuclear theory, however, also comes the need for novel…

Nuclear Theory · Physics 2024-11-26 R. Y. Cheng , K. Godbey , Y. B. Niu , Y. G. Ma , W. B. He , S. M. Wang

Multicomponent methods are a conceptually simple way to include nuclear quantum effects into quantum chemistry calculations. In multicomponent methods, the electronic molecular orbitals are described using the linear combination of atomic…

Chemical Physics · Physics 2022-12-02 Irina Samsonova , Gabrielle B. Tucker , Naresh Alaal , Kurt R. Brorsen

The method of Monte Carlo configuration interaction (MCCI) [1,2] is applied to the calculation of multipole moments. We look at the ground and excited state dipole moments in carbon monoxide. We then consider the dipole of NO, the…

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

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

Bandit methods for black-box optimisation, such as Bayesian optimisation, are used in a variety of applications including hyper-parameter tuning and experiment design. Recently, \emph{multi-fidelity} methods have garnered considerable…

Machine Learning · Statistics 2017-03-21 Kirthevasan Kandasamy , Gautam Dasarathy , Jeff Schneider , Barnabas Poczos

Efforts to describe nuclear structure and dynamics from first principles have advanced significantly in recent years. Exact methods for light nuclei are now able to include continuum degrees of freedom and treat structure and reactions on…

Background: Ab initio many-body methods whose numerical cost scales polynomially with the number of particles have been developed over the past fifteen years to tackle closed-shell mid-mass nuclei. Open-shell nuclei have been further…

Nuclear Theory · Physics 2018-06-27 Julien Ripoche , Thomas Duguet , Jean-Paul Ebran , Denis Lacroix

Stimulation methods that utilise more than one stimulation frequency have been developed for steady-state visual evoked potential (SSVEP) brain-computer interfaces (BCIs) with the purpose of increasing the number of targets that can be…

Neurons and Cognition · Quantitative Biology 2021-08-12 Jing Mu , Ying Tan , David B. Grayden , Denny Oetomo

Approximate full configuration interaction (FCI) calculations have recently become tractable for systems of unforeseen size thanks to stochastic and adaptive approximations to the exponentially scaling FCI problem. The result of an FCI…

Strongly Correlated Electrons · Physics 2017-10-25 Susi Lehtola , Norm M. Tubman , K. Birgitta Whaley , Martin Head-Gordon

The adoption of high-fidelity models for many-query optimization problems is majorly limited by the significant computational cost required for their evaluation at every query. Multifidelity Bayesian methods (MFBO) allow to include costly…

Machine Learning · Computer Science 2024-07-08 Francesco Di Fiore , Laura Mainini

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

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