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Unitary coupled cluster (UCC) theory offers a promising Hermitian alternative to conventional coupled cluster (CC) theory, but its practical implementation is hindered by the non-truncating nature of the Baker-Campbell-Hausdorff (BCH)…

Chemical Physics · Physics 2025-05-05 Justin T. Phillips , Lauren N. Koulias , Stephen H. Yuwono , A. Eugene DePrince

We extend our assessment of the potential of perturbative coupled cluster (CC) expansions for a test set of open-shell atoms and organic radicals to the description of quadruple excitations. Namely, the second- through sixth-order models of…

Chemical Physics · Physics 2016-05-17 Janus J. Eriksen , Devin A. Matthews , Poul Jørgensen , Jürgen Gauss

This study implements the full multicomponent third-order (MP3) and fourth-order (MP4) many-body perturbation theory methods for the first time. Previous multicomponent studies have only implemented a subset of the full contributions and…

Chemical Physics · Physics 2022-01-12 O. Jonathan Fajen , Kurt R. Brorsen

Tensor clustering, which seeks to extract underlying cluster structures from noisy tensor observations, has gained increasing attention. One extensively studied model for tensor clustering is the tensor block model, which postulates the…

Statistics Theory · Mathematics 2023-11-07 Yuchen Zhou , Yuxin Chen

Striving to define very accurate vertical transition energies, we perform both high-level coupled cluster (CC) calculations (up to CCSDTQP) and selected configuration interaction (sCI) calculations (up to several millions of determinants)…

We consider a fermionic system for which there exist a single-reference configuration-interaction (CI) expansion of the ground state wave function that converges, albeit not necessarily rapidly, with respect to excitation number. We show…

Strongly Correlated Electrons · Physics 2020-01-13 Dominic Bergeron

We resume the recent successes of the grid-based tensor numerical methods and discuss their prospects in real-space electronic structure calculations. These methods, based on the low-rank representation of the multidimensional functions and…

Numerical Analysis · Mathematics 2016-01-20 Venera Khoromskaia , Boris N. Khoromskij

Recently, Hohenstein et al[1] introduced tensor hypercontraction density fitting to decompose the rank-4 electron repulsion integral tensor as the product of five rank-2 tensors. In this paper, we use this methodology to construct an…

Chemical Physics · Physics 2012-09-14 Neil Shenvi , Helen Van Aggelen , Weitao Yang

Recent work has deployed linear combinations of unitaries techniques to reduce the cost of fault-tolerant quantum simulations of correlated electron models. Here, we show that one can sometimes improve upon those results with optimized…

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

Chemical Physics · Physics 2020-12-23 Jonathon P. Misiewicz , Justin M. Turney , Henry F. Schaefer , Alexander Yu. Sokolov

Novel implementations based on dense tensor storage are presented for the singlet-reference perfect quadruples (PQ) [Parkhill, Lawler, and Head-Gordon, J. Chem. Phys. 130, 084101 (2009)] and perfect hextuples (PH) [Parkhill and Head-Gordon,…

Strongly Correlated Electrons · Physics 2016-10-07 Susi Lehtola , John Parkhill , Martin Head-Gordon

In light of the recent discrepancies reported between fixed node diffusion Monte Carlo and local natural orbital coupled cluster with single, double and perturbative triples (CCSD(T)) methodologies for non-covalent interactions in large…

Chemical Physics · Physics 2024-11-22 S. Lambie , D. Kats , D. Usyvat , A. Alavi

We incorporate a canonical polyadic decomposition (CPD) based low-level solver as a means to accelerate the environment-level solver for the recently developed MPCC embedding framework. Using CPD, we both factorize the three dominant…

Chemical Physics · Physics 2026-02-19 Karl Pierce , Muhammad Talha Aziz , Avijit Shee , Fabian M. Faulstich

We introduce a black-box auxiliary field quantum Monte Carlo (AFQMC) approach to perform highly accurate electronic structure calculations using configuration interaction singles and doubles (CISD) trial states. This method consistently…

Electron repulsion integral tensor has ubiquitous applications in quantum chemistry calculations. In this work, we propose an algorithm which compresses the electron repulsion tensor into the tensor hypercontraction format with…

Numerical Analysis · Mathematics 2015-06-18 Jianfeng Lu , Lexing Ying

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

Theory of one-electron transition density matrices has been formulated within the time-independent coupled cluster method for the polarization propagator [R. Moszynski, P. S. \.Zuchowski, and B. Jeziorski, Coll. Czech. Chem. Commun. {\bf…

Chemical Physics · Physics 2014-09-25 Aleksandra M. Tucholska , Marcin Modrzejewski , Robert Moszynski

This paper introduces an extended tensor decomposition (XTD) method for model reduction. The proposed method is based on a sparse non-separated enrichment to the conventional tensor decomposition, which is expected to improve the…

Numerical Analysis · Mathematics 2023-11-07 Ye Lu , Satyajit Mojumder , Jiachen Guo , Yangfan Li , Wing Kam Liu

Spectral clustering is one of the most popular clustering methods. However, the high computational cost due to the involved eigen-decomposition procedure can immediately hinder its applications in large-scale tasks. In this paper we use…

Machine Learning · Computer Science 2023-01-24 Yongyu Wang

The global optimization of atomic clusters represents a fundamental challenge in computational chemistry and materials science due to the exponential growth of local minima with system size (i.e., the curse of dimensionality). We introduce…