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Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…

Materials Science · Physics 2022-01-11 Tina N. Mihm , Tobias Schäfer , Sai Kumar Ramadugu , Andreas Grüneis , James J. Shepherd

We have developed a relativistic coupled-cluster theory to incorporate nuclear spin-dependent interaction Hamiltonians perturbatively. This theory is ideal to calculate parity violating nuclear spin-dependent electric dipole transition…

Atomic Physics · Physics 2011-06-09 B. K. Mani , D. Angom

An externally corrected coupled cluster (CC) method, where an adaptive configuration interaction (ACI) wave function provides the external cluster amplitudes, named ACI-CC, is presented. By exploiting the connection between configuration…

Chemical Physics · Physics 2023-09-27 Gustavo J. R. Aroeira , Madeline M. Davis , Justin M. Turney , Henry F. Schaefer

We present a computationally efficient relativistic formulation of the equation-of-motion coupled-cluster method for the double electron attachment problem. In this work, the exact two-component Hamiltonian within the atomic mean-field…

Chemical Physics · Physics 2026-03-31 Sujan Mandal , Tamoghna Mukhopadhyay , Achintya Kumar Dutta

Fourth-order many-body corrections to matrix elements for atoms with one valence electron are derived. The obtained diagrams are classified using coupled-cluster-inspired separation into contributions from n-particle excitations from the…

Atomic Physics · Physics 2009-11-07 Andrei Derevianko , Erik D. Emmons

The correct calculation of formation enthalpy is one of the enablers of ab-initio computational materials design. For several classes of systems (e.g. oxides) standard density functional theory produces incorrect values. Here we propose the…

The S66x8 noncovalent interactions benchmark has been re-evaluated at the "sterling silver" level, using explicitly correlated MP2-F12 near the complete basis set limit, CCSD(F12*)/aug-cc-pVTZ-F12, and a (T) correction from conventional…

Chemical Physics · Physics 2022-10-31 Golokesh Santra , Emmanouil Semidalas , Nisha Mehta , Amir Karton , Jan M. L. Martin

We incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment…

Chemical Physics · Physics 2026-02-16 Avijit Shee , Fabian M. Faulstich , K. Birgitta Whaley , Lin Lin , Martin Head-Gordon

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)…

This paper proposes a method for designing BS clusters and cluster patterns for pair-wise BS coordination. The key idea is that each BS cluster is formed by using the 2nd-order Voronoi region, and the BS clusters are assigned to a specific…

Information Theory · Computer Science 2016-11-15 Jeonghun Park , Namyoon Lee , Robert W. Heath

The Slater-type F12 geminal lengthscales originally tuned for the second-order M{\o}ller-Plesset F12 method are too large for higher-order F12 methods formulated using the SP (diagonal fixed-coefficient spin-adapted) F12 ansatz. The new…

Chemical Physics · Physics 2025-10-13 Samuel R. Powell , Kshitijkumar A. Surjuse , Bimal Gaudel , Edward F. Valeev

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

We introduce a unitary coupled-cluster (UCC) ansatz termed $k$-UpCCGSD that is based on a family of sparse generalized doubles (D) operators which provides an affordable and systematically improvable unitary coupled-cluster wavefunction…

Quantum Physics · Physics 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

In quantum chemistry, one of the most important challenges is the static correlation problem when solving the electronic Schr\"odinger equation for molecules in the Born--Oppenheimer approximation. In this article, we analyze the tailored…

Numerical Analysis · Mathematics 2019-11-21 Fabian M. Faulstich , Andre Laestadius , Örs Legeza , Reinhold Schneider , Simen Kvaal

The impact of residual electron correlation beyond the equation-of-motion coupled-cluster singles and doubles approximation (EOM-CCSD) on positions and widths of electronic resonances is investigated. To establish a method that accomplishes…

Chemical Physics · Physics 2018-02-14 Thomas-C. Jagau

In this article we study the effects of higher body excitations in the relativistic CC calculations for atoms and ions with one valence electron using Fock-space CCSD, CCSD(T) and its unitary variants. The present study demonstrates that…

Atomic Physics · Physics 2009-11-13 Chiranjib Sur , Rajat K Chaudhuri

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

Block tensor decomposition (BTD) and canonical polyadic decomposition (CPD) are combined into a unified $O(N^3)$-scaling framework for second-order perturbation theory (PT2), demonstrated on MP2 and renormalized PT2 (rPT2). BTD constructs…

Chemical Physics · Physics 2026-05-28 Yueyang Zhang , Wei Wu , Peifeng Su

We analyze the accuracy of BCS-based approximations for calculating correlation energies and odd-even energy differences in 2-component fermionic systems with a small number of pairs. The analysis is focused on comparing BCS and projected…

Nuclear Theory · Physics 2009-01-16 N. Sandulescu , G. F. Bertsch

Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study…

Materials Science · Physics 2022-04-05 Verena A. Neufeld , Hong-Zhou Ye , Timothy C. Berkelbach