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A subsystem approach for obtaining electron binding energies in the valence region and apply it to the case of halide ions (X$^-$, X = F-At) in water. This approach is based on electronic structure calculations combining the relativistic…

We propose an approach to approximately implement the variational coupled cluster (VCC) theory on quantum computers, which struggles with exponential scaling of computational costs on classical computers. To this end, we employ expanding…

Quantum Physics · Physics 2024-06-12 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

The modified Cholesky decomposition is popular for inverse covariance estimation, but often needs pre-specification on the full information of variable ordering. In this work, we propose a block Cholesky decomposition (BCD) for estimating…

Methodology · Statistics 2023-08-21 Xiaoning Kang , Jiayi Lian , Xinwei Deng

A new computational framework for spinor-based relativistic exact two-component (X2C) calculations is developed using contracted basis sets with a spin-orbit contraction scheme. Generally contracted j-adapted basis sets using primitive…

Chemical Physics · Physics 2024-05-08 Chaoqun Zhang , Kirk A. Peterson , Kenneth G. Dyall , Lan Cheng

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

Downfolding coupled cluster (CC) techniques have recently been introduced into quantum chemistry as a tool for the dimensionality reduction of the many-body quantum problem. As opposed to earlier formulations in physics and chemistry based…

Quantum Physics · Physics 2022-03-23 Nicholas P. Bauman , Karol Kowalski

In this chapter we focus first on the theoretical methods and relevant computational approaches to calculate the electronic structure of atoms, molecules, and clusters containing heavy elements for which relativistic effects become…

Chemical Physics · Physics 2021-10-05 Simone Taioli , Stefano Simonucci

Concurrent multiscale methods play an important role in modeling and simulating materials with defects, aiming to achieve the balance between accuracy and efficiency. Atomistic-to-continuum (a/c) coupling methods, a typical class of…

Numerical Analysis · Mathematics 2025-02-27 Junfeng Lu , Hao Wang , Yangshuai Wang

Non-unitary theories are commonly seen in the classical simulations of quantum systems. Among these theories, the method of moments of coupled-cluster equations (MMCCs) and the ensuing classes of the renormalized coupled-cluster (CC)…

Quantum Physics · Physics 2022-12-13 Bo Peng , Karol Kowalski

Multicomponent systems are defined as chemical systems that require a quantum mechanical description of two or more different types of particles. Non-Born-Oppenheimer electron-nuclear interactions in molecules, electron-hole interactions in…

Chemical Physics · Physics 2015-10-21 Benjamin H. Ellis , Somil Aggarwal , Arindam Chakraborty

We present the theory and the implementation of a low-cost four-component relativistic equation of motion coupled cluster method for ionized states based on frozen natural spinors. A single threshold (natural spinor occupancy) can control…

Chemical Physics · Physics 2024-06-19 Kshitijkumar Surjuse , Somesh Chamoli , Malaya K. Nayak , Achintya Kumar Dutta

The cluster-in-molecule (CIM) local correlation approach with an accurate distant pair correlation energy correction is presented. For large systems, the inclusion of distant pair correlation energies is essential for the accurate…

Chemical Physics · Physics 2020-08-06 Zhigang Ni , Yang Guo , Frank Neese , Wei Li , Shuhua Li

We present a quantum linear response (qLR) approach within an active-space framework for computing indirect nuclear spin-spin coupling constants, a key ingredient in NMR spectra predictions. The method employs the unitary coupled cluster…

We present the implementation of a quadratically convergent Self-consistent field (QCSCF) algorithm based on an adaptive trust-radius optimization scheme for restricted open-shell Hartree-Fock (ROHF), restricted Hartree-Fock (RHF), and…

Chemical Physics · Physics 2022-01-12 Tommaso Nottoli , Jürgen Gauss , Filippo Lipparini

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

Chiral crystals show promise for spintronic technologies on account of their high spin selectivity, which has led to significant recent interest in quantitative characterization and first-principles prediction of their spin-optoelectronics…

Materials Science · Physics 2023-12-05 Christian Multunas , Andrew Grieder , Junqing Xu , Yuan Ping , Ravishankar Sundararaman

As a generalization of the two-dimensional Fourier transform (2D FT) and 2D fractional Fourier transform, the 2D nonseparable linear canonical transform (2D NsLCT) is useful in optics, signal and image processing. To reduce the digital…

Computer Vision and Pattern Recognition · Computer Science 2017-07-13 Soo-Chang Pei , Shih-Gu Huang

The curse of dimensionality (COD) limits the current state-of-the-art {\it ab initio} propagation methods for non-relativistic quantum mechanics to relatively few particles. For stationary structure calculations, the coupled-cluster (CC)…

Quantum Physics · Physics 2015-06-03 Simen Kvaal

We present a simple relativistic exact 2-component (X2C) Hamiltonian that models two-electron picture-change effects using Lehtola's superposition of atomic potentials (SAP) [S. Lehtola, J. Chem. Theory Comput. 15, 1593-1604 (2019)]. The…

Chemical Physics · Physics 2026-03-10 Kshitijkumar A. Surjuse , Edward F. Valeev

The relativistic coupled-cluster (RCC) method is a powerful many-body method, particularly in the evaluation of electronic wave functions of heavy atoms and molecules, and can be used to calculate various atomic and molecular properties.…

Atomic Physics · Physics 2019-12-09 Nanako Shitara , B. K. Sahoo , T. Watanabe , B. P. Das