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We investigate the electronic structure of a planar mononuclear Cu-based molecule [Cu(C$_6$H$_4$S$_2$)$_2$]$^z$ in two oxidation states ($z$$=$$-2$, $-$1) using density-functional theory (DFT) with Fermi-L\"owdin orbital (FLO)…

Mesoscale and Nanoscale Physics · Physics 2021-07-28 Anri Karanovich , Yoh Yamamoto , Koblar Alan Jackson , Kyungwha Park

We have investigated the efficacy of two recently proposed variations of the pair-natural-orbital approach to reducing the scaling of coupled cluster property calculations. In particular, we have extended our implementations of the PNO++…

Chemical Physics · Physics 2023-07-26 Ruhee D'Cunha , T. Daniel Crawford

Coupled cluster calculations are traditionally performed over Hartree-Fock reference orbitals (HF-CC methodology). However, it has been repeatedly argued in the literature that the use of a Kohn-Sham reference (KS-CC methodology) might…

Chemical Physics · Physics 2025-03-10 Zsolt Benedek , Paula Tímár , Tibor Szilvási , Gergely Barcza

Starting from realistic nuclear forces, the chiral N$^3$LO and JISP16, we have applied many-body perturbation theory (MBPT) to the structure of closed-shell nuclei, $^4$He and $^{16}$O. The two-body N$^3$LO interaction is softened by a…

Nuclear Theory · Physics 2019-11-07 Baishan Hu , Furong Xu , Zhonghao Sun , James P. Vary , Tong Li

We performed density-functional calculations to investigate the electronic structure of ZnO/GaN core/shell heterostructured nanowires (NWs) orientating along <0001> direction. The build-in electric filed arising from the charge…

Materials Science · Physics 2015-05-19 Zhenhai Wang , Yingcai Fan , Mingwen Zhao

We present a quantum computational framework using Hamiltonian Truncation (HT) for simulating real-time scattering processes in $(1+1)$-dimensional scalar $\phi^4$ theory. Unlike traditional lattice discretisation methods, HT approximates…

Quantum Physics · Physics 2025-05-08 James Ingoldby , Michael Spannowsky , Timur Sypchenko , Simon Williams , Matthew Wingate

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

Contributions from connected quintuple excitations in coupled cluster theory can reach the 0.5 kcal/mol range, important enough to matter in accurate computational thermochemistry, yet the very steep $\propto N^{12}$ CPU time scaling…

Chemical Physics · Physics 2026-05-22 Gregory H. Jones , Aditya Barman , Margarita Shepelenko , Jan M. L. Martin

Perdew-Zunger self-interaction correction (PZ-SIC) offers a route to remove self-interaction errors on an orbital-by-orbital basis. A recent formulation of PZ-SIC by Pederson, Ruzsinszky and Perdew proposes restricting the unitary…

Chemical Physics · Physics 2021-12-07 Carlos M. Diaz , Tunna Baruah , Rajendra R. Zope

The recently proposed natural orbital functional second-order M{\o}ller-Plesset (NOF-MP2) method is capableof achieving both dynamic and static correlation even for those systems with significant multiconfigurational character. We test its…

Chemical Physics · Physics 2019-06-12 Xabier Lopez , Mario Piris

We implement and benchmark the frozen core approximation, a technique commonly adopted in electronic structure theory to reduce the computational cost by means of mathematically fixing the chemically inactive core electron states. The…

Materials Science · Physics 2021-06-14 Victor Wen-zhe Yu , Jonathan Moussa , Volker Blum

We develop a local correlation variant of auxiliary field quantum Monte Carlo (AFQMC) that is based on local natural orbitals (LNO-AFQMC). In LNO-AFQMC, independent AFQMC calculations are performed for each localized occupied orbital using…

Chemical Physics · Physics 2023-08-25 Jo S. Kurian , Hong-Zhou Ye , Ankit Mahajan , Timothy C. Berkelbach , Sandeep Sharma

We present a method to approximate post-Hartree-Fock correlation energies by using approximate natural orbitals obtained by the random phase approximation (RPA). We demonstrate the method by applying it to the helium atom, the hydrogen and…

Chemical Physics · Physics 2021-03-22 Benjamin Ramberger , Zoran Sukurma , Tobias Schäfer , Georg Kresse

In this study, we propose a quantum-classical hybrid scheme for performing orbital-free density functional theory (OFDFT) using probabilistic imaginary-time evolution (PITE), designed for the era of fault-tolerant quantum computers (FTQC),…

Quantum Physics · Physics 2024-07-24 Yusuke Nishiya , Hirofumi Nishi , Taichi Kosugi , Yu-ichiro Matsushita

The energy and analytic gradient are developed for FMO combined with the Hartree-Fock method augmented with three empirical corrections (HF-3c). The auxiliary basis set approach to FMO is extended to perform pair interaction energy…

Chemical Physics · Physics 2018-08-01 Dmitri G. Fedorov , Jimmy C. Kromann , Jan H. Jensen

We find an unexpected scaling in the correlation energy of artificial atoms, i.e., harmonically confined two-dimensional quantum dots. The scaling relation is found through extensive numerical examinations including Hartree-Fock,…

Mesoscale and Nanoscale Physics · Physics 2015-04-28 Alexander Odriazola , Mikko M Ervasti , Ilja Makkonen , Alain Delgado , Augusto González , Esa Räsänen , Ari Harju

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

We present a near-linear scaling formulation of the explicitly-correlated coupled-cluster singles and doubles with perturbative triples method (CCSD(T)$_{\overline{\text{F12}}}$) for high-spin states of open-shell species. The approach is…

Chemical Physics · Physics 2024-07-30 Ashutosh Kumar , Frank Neese , Edward F. Valeev

Despite the tremendous advances made by the ab initio theory of electronic structure of atoms and molecules, its applications are still not possible for very large systems. Therefore, semi-empirical model Hamiltonians based on the…

Atomic and Molecular Clusters · Physics 2009-11-13 Sridhar Sahu , Alok Shukla

In quantum chemistry, self-consistent field (SCF) algorithms define a nonlinear optimization problem, with both continuous and discrete components. In this work, we derive Hartree-Fock-inspired SCF algorithms that can be exactly written as…

Quantum Physics · Physics 2025-06-05 Alexis Ralli , Tim Weaving , Peter V. Coveney , Peter J. Love