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In this work, we developed an efficient approach to compute ensemble averages in systems with pairwise-additive energetic interactions between the entities. Methods involving full enumeration of the configuration space result in exponential…

Biomolecules · Quantitative Biology 2020-10-13 Arun V. Sathanur , Nathan A. Baker

Coupled cluster theory is a vital cornerstone of electronic structure theory and is being applied to ever-larger systems. Stochastic approaches to quantum chemistry have grown in importance and offer compelling advantages over traditional…

In this paper, we address technical difficulties that arise when applying Markov chain Monte Carlo (MCMC) to hierarchical models designed to perform clustering in the space of latent parameters of subject-wise generative models.…

Quantitative Methods · Quantitative Biology 2020-12-15 Yu Yao , Klaas E. Stephan

We present two efficient and intruder-free methods for treating dynamic correlation on top of general multi-configuration reference wave functions---including such as obtained by the density matrix renormalization group (DMRG) with large…

Chemical Physics · Physics 2016-09-13 Sandeep Sharma , Gerald Knizia , Sheng Guo , Ali Alavi

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…

Chemical Physics · Physics 2020-02-19 Robert J. Anderson , Toru Shiozaki , George H. Booth

Ensemble Kalman methods solve problems in domains such as filtering and inverse problems with interacting particles that evolve over time. For computationally expensive problems, the cost of attaining a high accuracy quickly becomes…

Numerical Analysis · Mathematics 2025-02-18 Arne Bouillon , Toon Ingelaere , Giovanni Samaey

The tailored coupled cluster (TCC) approach is a promising ansatz that preserves the simplicity of single-reference coupled cluster theory, while incorporating a multi-reference wave function through amplitudes obtained from a preceding…

Chemical Physics · Physics 2021-01-07 Maximilian Mörchen , Leon Freitag , Markus Reiher

In online clustering problems, there is often a large amount of uncertainty over possible cluster assignments that cannot be resolved until more data are observed. This difficulty is compounded when clusters follow complex distributions, as…

Machine Learning · Statistics 2026-04-17 Connie Trojan , Pavel Myshkov , Paul Fearnhead , James Hensman , Tom Minka , Christopher Nemeth

In this work, we investigate the possibility of improving multireference-driven coupled cluster (CC) approaches with an algorithm that iteratively combines complete active space (CAS) calculations with tailored CC and externally corrected…

Chemical Physics · Physics 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

We propose a streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

Strongly Correlated Electrons · Physics 2021-07-28 Ke Liao , Thomas Schraivogel , Hongjun Luo , Daniel Kats , Ali Alavi

Multilevel Monte Carlo (MLMC) has become an important methodology in applied mathematics for reducing the computational cost of weak approximations. For many problems, it is well-known that strong pairwise coupling of numerical solutions in…

Numerical Analysis · Mathematics 2022-10-11 Neil K. Chada , Håkon Hoel , Ajay Jasra , Georgios E. Zouraris

We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment…

Chemical Physics · Physics 2024-11-13 Avijit Shee , Fabian M. Faulstich , Birgitta Whaley , Lin Lin , Martin Head-Gordon

We introduce a novel class of coupled cluster (CC) methods that leverage the seniority concept to enhance efficiency and accuracy in electronic structure calculations. While existing approaches, such as the pair coupled cluster doubles…

We review efficient Monte Carlo methods for simulating quantum systems which couple to a dissipative environment. A brief introduction of the Caldeira-Leggett model and the Monte Carlo method will be followed by a detailed discussion of…

Statistical Mechanics · Physics 2009-11-11 Philipp Werner , Matthias Troyer

The small magnitude and long-range character of non-covalent interactions pose a significant challenge for computational quantum chemical and electronic-structure methods alike. State-of-the-art coupled cluster (CC) theory and…

Chemical Physics · Physics 2026-01-22 S. Lambie , P. López-Ríos , D. Kats , Ali Alavi

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

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

Development of exponentially scaling methods has seen great progress in tackling larger systems than previously thought possible. One such technique, full configuration interaction quantum Monte Carlo, is a useful algorithm that allows…

Strongly Correlated Electrons · Physics 2016-08-23 Norm M. Tubman , Joonho Lee , Tyler Y. Takeshita , Martin Head-Gordon , K. Birgitta Whaley

Coupled cluster methods are widely regarded as the gold standard of computational quantum chemistry as they are perceived to offer the best compromise between computational cost and a high-accuracy resolution of the ground state eigenvalue…

Numerical Analysis · Mathematics 2025-12-03 Muhammad Hassan , Yvon Maday

High-order perturbative $\textit{ab initio}$ calculations are challenging due to the rapidly growing configuration space and the difficulty of assessing convergence. In this letter, we introduce perturbation theory quantum Monte Carlo…

Nuclear Theory · Physics 2026-05-06 Xin Zhen , Rongzhe Hu , Junchen Pei , Furong Xu