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We propose a relativistic unitary coupled cluster (UCC) expectation value approach for computing first-order properties of heavy-element systems. Both perturbative (UCC3) and non-perturbative (qUCC) commutator-based formulations are applied…

Chemical Physics · Physics 2026-02-03 Kamal Majee , Somesh Chamoli , Malaya K. Nayak , Achintya Kumar Dutta

This paper introduces a new computational framework to derive electromagnetic field derivatives with respect to multiple design parameters up to any order with the Finite-Difference Time-Domain (FDTD) technique. Specifically, only one FDTD…

Signal Processing · Electrical Eng. & Systems 2019-10-23 Kae-An Liu , Costas D. Sarris

We set up the framework for the calculation of electric dipole moments (EDMs) of light nuclei using the systematic expansion provided by chiral effective field theory (EFT). We take into account parity (P) and time-reversal (T) violation…

High Energy Physics - Phenomenology · Physics 2011-12-12 J. de Vries , R. Higa , C. -P. Liu , E. Mereghetti , I. Stetcu , R. G. E. Timmermans , U. van Kolck

Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…

Chemical Physics · Physics 2022-10-06 Karthik Gururangan , J. Emiliano Deustua , Jun Shen , Piotr Piecuch

In this article, the molecular permanent electric dipole moments and components of static dipole polarizabilities for the electronic ground state of singly charged aluminum monohalides are reported. The coupled-cluster method by considering…

Atomic Physics · Physics 2024-06-18 Ankush Thakur , Renu Bala , H. S. Nataraj , V. S. Prasannaa

High-order harmonic generation (HHG) results from strong-field laser matter interaction and it is one of the main processes that are used to extract electron structural and dynamical information about the atomic or molecular targets with…

The relativistic multiconfiguration Dirac-Hartree-Fock (MCDHF) and the non-relativistic multiconfiguration Hartree-Fock (MCHF) methods have been employed to calculate the magnetic dipole and electric quadrupole hyperfine structure constants…

Heavy polar diatomic molecules are currently among the most promising probes of fundamental physics. Constraining the electric dipole moment of the electron (eEDM), in order to explore physics beyond the Standard Model, requires a synergy…

Atomic Physics · Physics 2018-04-18 M Abe , V S Prasannaa , B P Das

In the framework of the computational determination of highly-accurate vertical excitation energies in small organic compounds, we explore the possibilities offered by the equation-of-motion formalism relying on the approximate fourth-order…

We revisited the electronic structure parameters used to interpret the hyperfine structure of neutral polonium. We used a computational scheme that treats relativistic and high-order electronic correlation effects within the coupled cluster…

Atomic Physics · Physics 2024-03-08 Leonid V. Skripnikov , Anatoly E. Barzakh

Coupled cluster with single, double, and perturbative triple excitations [CCSD(T)] has been extensively employed as the reference method in benchmarking different quantum chemistry methods. In this work, we test the accuracy of CCSD(T)…

Chemical Physics · Physics 2021-07-21 Xiangyue Liu , Laura McKemmish , Jesús Pérez-Ríos

We describe our efforts of the past few years to create a large set of more than 500 highly-accurate vertical excitation energies of various natures ($\pi \to \pi^*$, $n \to \pi^*$, double excitation, Rydberg, singlet, doublet, triplet,…

The analytic gradient theory for both iterative and non-iterative coupled-cluster approximations that include connected quadruple excitations is presented. These methods include, in particular, CCSDT(Q), which is an analog of the well-known…

Chemical Physics · Physics 2025-03-26 Devin A. Matthews

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)…

We recently proposed a novel approach to converging electronic energies equivalent to high-level coupled-cluster (CC) computations by combining the deterministic CC($P$;$Q$) formalism with the stochastic configuration interaction (CI) and…

Chemical Physics · Physics 2021-03-23 J. Emiliano Deustua , Jun Shen , Piotr Piecuch

We present a general approach within the relativistic coupled-cluster theory framework to calculate exactly the first order wave functions due to any rank perturbation operators. Using this method, we calculate the static dipole and…

Atomic Physics · Physics 2009-11-13 B. K. Sahoo

Simulating molecules using the Variational Quantum Eigensolver method is one of the promising applications for NISQ-era quantum computers. Designing an efficient ansatz to represent the electronic wave function is crucial in such…

Chemical Physics · Physics 2022-05-09 Dmitry A. Fedorov , Yuri Alexeev , Stephen K. Gray , Matthew Otten

We introduce a non-iterative energy correction, added on top of the rank-reduced coupled-cluster method with single, double, and triple substitutions, that accounts for excitations excluded from the parent triple excitation subspace. The…

Chemical Physics · Physics 2022-01-06 Michał Lesiuk

The multiconfiguration Dirac-Hartree-Fock (MCDHF) method has been employed to calculate atomic electric dipole moments (EDM) of 225^Ra, 199^Hg, and 171^Yb. For the calculations of the matrix elements we extended the relativistic atomic…

Atomic Physics · Physics 2013-12-24 Laima Radziute , Gediminas Gaigalas , Per Jonsson , Jacek Biero

A variational solution procedure is reported for the many-particle no-pair Dirac-Coulomb-Breit Hamiltonian aiming at a parts-per-billion (ppb) convergence of the atomic and molecular energies, described within the fixed nuclei…

Quantum Physics · Physics 2024-06-19 Péter Jeszenszki , Dávid Ferenc , Edit Mátyus