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The study of isolated defects in solids is a natural target for classical or quantum embedding methods that treat the defect at a high level of theory and the rest of the solid at a lower level of theory. Here, in the context of…

Materials Science · Physics 2023-01-25 Bryan T. G. Lau , Brian Busemeyer , Timothy C. Berkelbach

The recent development of the density matrix renormalization group (DMRG) method in multireference quantum chemistry makes it practical to evaluate static correlation in a large active space, while dynamic correlation provides a critical…

Strongly Correlated Electrons · Physics 2020-08-20 Zhen Luo , Yingjin Ma , Xicun Wang , Haibo Ma

By combining extrapolated selected configuration interaction (sCI) energies obtained with the CIPSI (Configuration Interaction using a Perturbative Selection made Iteratively) algorithm with the recently proposed short-range…

Chemical Physics · Physics 2020-06-05 Emmanuel Giner , Anthony Scemama , Julien Toulouse , Pierre-François Loos

We present a comprehensive theoretical study of the physical phenomena that determine the relative energies of the three of the lowest electronic states of each of the square-planar copper complexes $\cucl$, $\cunh$ and $\cuwater$, and…

Strongly Correlated Electrons · Physics 2018-06-14 Emmanuel Giner , David Tew , Yann Garniron , Ali Alavi

Neutral uranium (U I) is a very difficult atom for theoretical calculations due to a large number of valence electrons, six, strong valence-valence and valence-core correlations, high density of states, and relativistic effects.…

Atomic Physics · Physics 2020-10-14 Igor M. Savukov

The nuclear-electronic orbital (NEO) approach incorporates nuclear quantum effects into quantum chemistry calculations by treating specified nuclei quantum mechanically, equivalently to the electrons. Within the NEO framework, excited…

Chemical Physics · Physics 2025-03-19 Christopher L. Malbon , Sharon Hammes-Schiffer

The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals…

Computational Physics · Physics 2021-12-22 Daniel S. Levine , Diptarka Hait , Norm M. Tubman , Susi Lehtola , K. Birgitta Whaley , Martin Head-Gordon

We present a quantum-classical hybrid algorithm for calculating the ground state and its energy of the quantum many-body Hamiltonian by proposing an adaptive construction of a quantum state for the quantum-selected configuration interaction…

Quantum Physics · Physics 2024-12-12 Yuya O. Nakagawa , Masahiko Kamoshita , Wataru Mizukami , Shotaro Sudo , Yu-ya Ohnishi

Noise and errors are inevitable parts of any practical implementation of a quantum computer. As a result, large-scale quantum computation will require ways to detect and correct errors on quantum information. Here, we present such a quantum…

Numerical simulations of crystal defects are necessarily restricted to finite computational domains, supplying artificial boundary conditions that emulate the effect of embedding the defect in an effectively infinite crystalline…

Numerical Analysis · Mathematics 2016-05-25 V. Ehrlacher , C. Ortner , A. V. Shapeev

Configuration interaction (CI) calculations in atoms with two valence electrons, carried out in the V(N-2) Hartree-Fock potential of the core, are corrected for core-valence interactions using many-body perturbation theory (MBPT). Two…

Atomic Physics · Physics 2009-11-07 I. M. Savukov , W. R. Johnson

Quantum-selected configuration interaction (QSCI) utilizes an input quantum state on a quantum device to select important bases (electron configurations in quantum chemistry) that define a subspace in which to diagonalize a target…

Quantum Physics · Physics 2025-10-22 Mathias Mikkelsen , Yuya O. Nakagawa

We present the concept, derivation, and implementation of dynamical configuration interaction, a quantum embedding theory that combines Green's function methodology with the many-body wave function. In a strongly-correlated active space, we…

Chemical Physics · Physics 2019-04-03 Marc Dvorak , Patrick Rinke

Determination of defect ionization energy in low-dimensional semiconductors has been a long-standing unsolved problem in first-principles defect calculations because the commonly used methods based on jellium model introduce an unphysical…

Materials Science · Physics 2020-07-15 Guo-jun Zhu , Xin-Gao Gong , Ji-Hui Yang

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

We present a relativistic correction scheme to improve the accuracy of 1s core-level binding energies calculated from Green's function theory in the $GW$ approximation, which does not add computational overhead. An element-specific…

Chemical Physics · Physics 2020-09-23 Levi Keller , Volker Blum , Patrick Rinke , Dorothea Golze

Self-interaction (SI) error, which results when exchange-correlation contributions to the total energy are approximated, limits the reliability of many density functional approximations. The Perdew-Zunger SI correction (PZSIC), when applied…

Excited states exhibiting double excitation character are notoriously difficult to model using conventional single-reference methods, such as adiabatic time-dependent density-functional theory (TD-DFT) or equation-of-motion coupled cluster…

The recently developed semistochastic heat-bath configuration interaction (SHCI) method is a systematically improvable selected configuration interaction plus perturbation theory method capable of giving essentially exact energies for…

Chemical Physics · Physics 2020-10-01 Yuan Yao , Emmanuel Giner , Junhao Li , Julien Toulouse , C. J. Umrigar

We present unrestricted Hartree Fock method coupled with configuration interaction (CI) method (URHF-CI) suitable for the calculation of ground and excited states of large number of electrons localized by complex gate potentials in…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Ramin M. Abolfath , Pawel Hawrylak