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A novel approach to rapidly converging high-level coupled-cluster (CC) energetics in an automated fashion is proposed. The key idea is an adaptive selection of the excitation manifolds defining higher-than-two-body components of the cluster…

Chemical Physics · Physics 2023-08-25 Karthik Gururangan , Piotr Piecuch

Coupled cluster theory produced arguably the most widely used high-accuracy computational quantum chemistry methods. Despite the approach's overall great computational success, its mathematical understanding is so far limited to results…

Algebraic Geometry · Mathematics 2024-03-29 Fabian M. Faulstich , Mathias Oster

Given a set of variables and the correlations among them, we develop a method for finding clustering among the variables. The method takes advantage of information implicit in higher-order (not just pairwise) correlations. The idea is to…

Statistical Mechanics · Physics 2015-05-13 L. S. Schulman

While limited coupled cluster theory is \textit{formally} nonvariational, it is not broadly appreciated whether this is a major issue \textit{in practice}. We carried out a detailed comparison with \textit{de facto} full CI energies for a…

Chemical Physics · Physics 2024-10-03 Jan M. L. Martin , Emmanouil Semidalas

The chemistry community has long sought the exact relationship between the conventional and the unitary coupled cluster ansatz for a single-reference system, especially given the interest in performing quantum chemistry on quantum…

Quantum Physics · Physics 2022-01-31 James K. Freericks

We study the application of various forms of the coupled cluster method to systems with paired fermions. The novel element of the analysis is the study of the breaking and eventual restoration of particle number in the CCM variants. We…

Quantum Physics · Physics 2010-11-24 Chris Snape , Niels R. Walet

We consider the sampling of the coupled cluster expansion within stochastic coupled cluster theory. Observing the limitations of previous approaches due to the inherently non-linear behaviour of a coupled cluster wavefunction representation…

Chemical Physics · Physics 2018-08-14 Charles J. C. Scott , Alex J. W. Thom

The accurate description of nuclear quantum effects, such as zero-point energy, is important for modeling a wide range of chemical and biological processes. Within the nuclear-electronic orbital (NEO) approach, such effects are incorporated…

Chemical Physics · Physics 2022-09-07 Fabijan Pavošević , Sharon Hammes-Schiffer

One method of representing a high-rank tensor as a (hyper-)product of lower-rank tensors is the tensor hypercontraction (THC) method of Hohenstein et al. This strategy has been found to be useful for reducing the polynomial scaling of…

Chemical Physics · Physics 2025-03-26 Avdhoot Datar , Devin A. Matthews

In this paper we extend the rank-reduced coupled-cluster formalism to the calculation of non-iterative energy corrections due to quadruple excitations. There are two major components of the proposed formalism. The first is an approximate…

Chemical Physics · Physics 2022-11-11 Michał Lesiuk

Density functional theory (DFT)-based simulations of materials have first-principles accuracy, but are very computationally expensive. For simulating various properties of multi-component alloys, the cluster expansion (CE) technique has…

Materials Science · Physics 2026-04-01 Jacob Jeffries , Bochuan Sun , Enrique Martinez

The second-order reduced density matrix method (the RDM method) has performed well in determining energies and properties of atomic and molecular systems, achieving coupled-cluster singles and doubles with perturbative triples (CC SD(T))…

Strongly Correlated Electrons · Physics 2012-07-23 James S. M. Anderson , Maho Nakata , Ryo Igarashi , Katsuki Fujisawa , Makoto Yamashita

In a series of two articles, we propose a comprehensive mathematical framework for Coupled-Cluster-type methods. In this second part, we analyze the nonlinear equations of the single-reference Coupled-Cluster method using topological degree…

Numerical Analysis · Mathematics 2023-03-28 Mihály A. Csirik , Andre Laestadius

Accurate yet efficient modeling of chemical systems with pronounced static correlation in their excited states remains a significant challenge in quantum chemistry, as most electronic structure methods that can adequately capture static…

Chemical Physics · Physics 2025-03-07 Sylvia J. Bintrim , Kevin Carter-Fenk

We investigate the efficient combination of the canonical polyadic decomposition (CPD) and tensor hyper-contraction (THC) approaches. We first present a novel low-cost CPD solver which leverages a precomputed THC factorization of an…

Chemical Physics · Physics 2025-05-28 Karl Pierce , Miguel Morales

High-order clustering aims to identify heterogeneous substructures in multiway datasets that arise commonly in neuroimaging, genomics, social network studies, etc. The non-convex and discontinuous nature of this problem pose significant…

Methodology · Statistics 2022-10-11 Rungang Han , Yuetian Luo , Miaoyan Wang , Anru R. Zhang

Coupled-cluster theories can be used to compute ab initio electronic correlation energies of real materials with systematically improvable accuracy. However, the widely-used coupled cluster singles and doubles plus perturbative triples…

Materials Science · Physics 2024-03-01 Nikolaos Masios , Andreas Irmler , Tobias Schäfer , Andreas Grüneis

With the aggressive scaling of VLSI technology, the explosion of layout patterns creates a critical bottleneck for DFM applications like OPC. Pattern clustering is essential to reduce data complexity, yet existing methods struggle with…

Hardware Architecture · Computer Science 2025-12-16 Shuo Liu

The pair-coupled-cluster doubles (pCCD) method has emerged as a viable approach for quantum-chemical studies of strongly correlated systems. Despite its lower formal scaling (O(N$^4$)) compared to other versions of coupled cluster (CC)…

Chemical Physics · Physics 2026-04-17 Rahul Chakraborty , Paweł Tecmer

Accurately resolving many-body satellite features in molecular core-level spectra requires theoretical approaches that capture electron correlation both efficiently and systematically. The recently developed time-dependent double…

Quantum Physics · Physics 2026-05-12 Vibin Abraham , Priyabrata Senapati , Himadri Pathak , Bo Peng