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We present a reduced-cost equation-of-motion coupled-cluster method for excited states, built on a new state-specific frozen natural orbital (SS-FNO) framework. This approach enables systematic and controllable truncation of the virtual…

Chemical Physics · Physics 2025-07-24 Amrita Manna , Achintya Kumar Dutta

We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…

Chemical Physics · Physics 2022-09-13 Tommaso Giovannini , Henrik Koch

We introduce affordable computational strategies for calculating orbital and pair-orbital energies in atomic and molecular systems. Our methods are based on the pair Coupled Cluster Doubles (pCCD) ansatz and its orbital-optimized variant.…

Chemical Physics · Physics 2025-02-06 Seyedehdelaram Jahani , Somayeh Ahmadkhani , Katharina Boguslawski , Paweł Tecmer

A new method for the nonperturbative solution of quantum field theories is described. The method adapts the exponential-operator technique of the standard many-body coupled-cluster method to the Fock-space eigenvalue problem for light-front…

High Energy Physics - Phenomenology · Physics 2015-05-30 J. R. Hiller , S. S. Chabysheva

The issue of orbital relaxation in computational core-hole spectroscopy, specifically x-ray absorption, has been a major problem for methods such as equation-of-motion coupled cluster with singles and doubles (EOM-CCSD). The…

Chemical Physics · Physics 2025-03-26 Megan Simons , Devin A. Matthews

Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…

Chemical Physics · Physics 2026-02-05 Prateek Vaish , Brenda Rubenstein

Modeling charge transfer well can require treating post-excitation orbital relaxations and handling medium to large molecules in realistic environments. By combining a state-specific correlation treatment with such orbital relaxations,…

Chemical Physics · Physics 2025-07-28 Harrison Tuckman , Eric Neuscamman

We present a spin-free, size-extensive, and size-consistent coupled cluster method based on a generalised normal ordered exponential ansatz. This approach is a natural generalisation of single-reference coupled cluster theory for arbitrary…

Chemical Physics · Physics 2025-07-21 Nicholas Lee , David P. Tew

An efficient approach to calculate approximate pure-state and transition reduced density matrices in the framework of the multireference relativistic Fock-space coupled cluster (FS CC) theory is proposed. The method is based on the…

Computational Physics · Physics 2025-06-12 Alexander V. Oleynichenko , Andrei Zaitsevskii , Leonid V. Skripnikov , Ephraim Eliav

Ab initio calculations face the challenge of describing a complex multiscale quantum many-body system. The nuclear wave function has both strong short-range correlations and long-range contributions. Natural orbitals provide a means of…

Nuclear Theory · Physics 2017-04-11 Chrysovalantis Constantinou

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

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

Orbital relaxation of the core region is a primary source of error in the computation of core ionization and core excitation energies. Recently, Transition-Potential Coupled Cluster (TP-CC) methods have been used to explicitly treat orbital…

Chemical Physics · Physics 2025-03-17 Alexis A. A. Delgado , Devin A. Matthews

We present the theory, implementation, and benchmark results for a frozen natural spinors-based lower scaling four-component relativistic coupled cluster method. The natural spinors are obtained by diagonalizing the one-body reduced density…

Chemical Physics · Physics 2022-06-15 Somesh Chamoli , Kshitijkumar Surjuse , Malaya K. Nayak , Achintya Kumar Dutta

The original formulation (Phys. Rev. Lett. 119, 063002, 2017) of the natural orbital functional - second-order M{\o}ller-Plesset (NOF-MP2) method is based on the MP2 that uses the canonical Hartree-Fock molecular orbitals. The current work…

Chemical Physics · Physics 2018-08-22 Mario Piris

The resolution of Brownian motion in simulations of micro-particle suspensions can be crucial to reproducing the correct dynamics of individual particles, as well as providing an accurate characterisation of suspension properties. Including…

Fluid Dynamics · Physics 2015-06-16 Eric E. Keaveny

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

A variant of coupled-cluster theory is described here, wherein the degrees of freedom are fluctuations of fragments between internally correlated states. The effects of intra-fragment correlation on the inter-fragment interaction are…

Chemical Physics · Physics 2019-05-24 Yuhong Liu , Anthony D. Dutoi

Five time-dependent orbital optimized coupled-cluster (TD-ooCC) methods, of which four can converge to the complete active space self-consistent-field method, are presented for fermion-mixtures with arbitrary fermion kinds and numbers.…

Chemical Physics · Physics 2024-07-08 Haifeng Lang , Takeshi Sato

The problem of orbital relaxation in computational core-hole spectroscopies, including x-ray absorption and x-ray photoionization, has long plagued linear response approaches, including equation-of-motion coupled cluster with singles and…

Chemical Physics · Physics 2025-03-26 Megan E. Simons , Devin A. Matthews
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