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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

In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

Wave functions based on electron-pair states provide inexpensive and reliable models to describe quantum many-body problems containing strongly-correlated electrons, given that broken-pair states have been appropriately accounted for by,…

Chemical Physics · Physics 2021-03-17 Artur Nowak , Ors Legeza , Katharina Boguslawski

Doubly occupied configuration interaction (DOCI) with optimized orbitals often accurately describes strong correlations while working in a Hilbert space much smaller than that needed for full configuration interaction. However, the scaling…

Chemical Physics · Physics 2016-02-25 Thomas M. Henderson , Ireneusz W. Bulik , Tamar Stein , Gustavo E. Scuseria

L-edge X-ray absorption spectra for first-row transition metal complexes are obtained from relativistic equation-of-motion singles and doubles coupled-cluster (EOM-CCSD) calculations that make use of the core-valence separation (CVS)…

Low-scaling electron correlation theory based on the pair natural orbital approximation, PNO-CCSD(T), has become a powerful computational tool. Motivated by the recent discovery of large errors for organometallic molecules, we assess the…

Chemical Physics · Physics 2023-10-10 Reka A. Horvath , Kesha Sorathia , Isabelle Saint , David P. Tew

We propose an orbital optimized method for unitary coupled cluster theory (OO-UCC) within the variational quantum eigensolver (VQE) framework for quantum computers. OO-UCC variationally determines the coupled cluster amplitudes and also…

Strongly Correlated Electrons · Physics 2020-09-23 Wataru Mizukami , Kosuke Mitarai , Yuya O. Nakagawa , Takahiro Yamamoto , Tennin Yan , Yu-ya Ohnishi

The projection-based quantum embedding method is applied to electronically excited states of valence, Rydberg, and charge-transfer character, valence- and core-ionized states, as well as bound and temporary radical anions. We embed…

Chemical Physics · Physics 2021-06-10 Valentina Parravicini , Thomas-C. Jagau

The double ionization potential (DIP) equation-of-motion (EOM) coupled-cluster (CC) method with a full treatment of 4-hole-2-particle (4$h$-2$p$) correlations and triply excited clusters, abbreviated as DIP-EOMCCSDT(4$h$-2$p$), and its…

Chemical Physics · Physics 2025-02-12 Karthik Gururangan , Achintya Kumar Dutta , Piotr Piecuch

The simultaneous treatment of static and dynamical correlations in strongly-correlated electron systems is a critical challenge. In particular, finding a universal scheme for identifying a single-particle orbital basis that minimizes the…

Quantum Physics · Physics 2024-08-07 Ke Liao , Lexin Ding , Christian Schilling

We formulate a parity-mixed coupled-cluster (PM-CC) approach for high-precision calculations of parity non-conserving amplitudes in mono-valent atoms. Compared to the conventional formalism which uses parity-proper (PP) one-electron…

Atomic Physics · Physics 2022-02-16 H. B. Tran Tan , Di Xiao , A. Derevianko

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

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

The time-dependent multiconfiguration self-consistent-field method based on the occupation-restricted multiple active space model is proposed (TD-ORMAS) for multielectron dynamics in intense laser fields. Extending the previously proposed…

Atomic Physics · Physics 2015-06-23 Takeshi Sato , Kenichi L. Ishikawa

We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

Chemical Physics · Physics 2015-08-17 Inkoo Kim , Shane M. Parker , Toru Shiozaki

Time-dependent equation-of-motion coupled cluster (TD-EOM-CC) is used to simulate impulsive stimulated x-ray Raman scattering (ISXRS) of ultrashort laser pulses by neon, carbon monoxide, pyrrole, and p-aminophenol. The TD-EOM-CC equations…

Chemical Physics · Physics 2023-10-10 Alice Balbi , Andreas S. Skeidsvoll , Henrik Koch

Real-time coupled cluster (CC) methods have several advantages over their frequency-domain counterparts, namely, response and equation of motion CC theories. Broadband spectra, strong fields, and pulse manipulation allow for the simulation…

Chemical Physics · Physics 2023-08-04 Benjamin G. Peyton , Zhe Wang , T. Daniel Crawford

In this work, we develop a mathematical framework for a Selected Configuration Interaction (SCI) algorithm within a bi-orthogonal basis for transcorrelated (TC) calculations. The bi-orthogonal basis used here serves as the equivalent of the…

Chemical Physics · Physics 2023-06-22 Abdallah Ammar , Anthony Scemama , Emmanuel Giner

We present the quantum-selected configuration interaction-tailored coupled-cluster (QSCI-TCC) method, a hybrid quantum-classical scheme that tailors coupled-cluster (CC) theory with a quantum-selected configuration interaction (QSCI) wave…

Chemical Physics · Physics 2025-06-23 Luca Erhart , Yuichiro Yoshida , Wataru Mizukami

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer