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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

Detecting and controlling nuclear spin nano-ensembles is crucial for the further development of nuclear magnetic resonance (NMR) spectroscopy and for the emerging solid state quantum technology. Here we present the fabrication of a…

The RPA long range correlations are known to play a significant role in understanding the depletion of single particle-hole states observed in (e, e') and (e, e'p) measurements. Here the Random Phase Approximation (RPA) theory, implemented…

Nuclear Theory · Physics 2009-11-11 M. Dupuis , S. Karataglidis , E. Bauge , J. P. Delaroche , D. Gogny

We present the implementation of relativistic coupled cluster quadratic response theory (QR-CC), following our development of relativistic equation of motion coupled cluster quadratic response theory (QR-EOMCC) [X. Yuan et al., J. Chem.…

Chemical Physics · Physics 2025-11-17 Xiang Yuan , Loïc Halbert , Lucas Visscher , André Severo Pereira Gomes

A hierarchy of wavefunction composite methods (cWFT), based on G4- type cWFT methods available for elements H through Rn, was recently reported by Semidalas and Martin [J. Chem. Theor. Comput. 2020, 16, 4238]. We extend this hierarchy by…

Chemical Physics · Physics 2021-02-09 Emmanouil Semidalas , Jan M. L. Martin

The random phase approximation (RPA) has emerged as a prominent first-principles method in material science, particularly to study the adsorption and chemisorption of small molecules on surfaces. However, its widespread application is…

Materials Science · Physics 2025-09-01 Edoardo Spadetto , Pier Herman Theodoor Philipsen , Arno Förster , Lucas Visscher

For many-body methods such as MCSCF and CASSCF, in which the number of one-electron orbitals are optimized and independent of basis set used, there are no problems with using plane-wave basis sets. However, for methods currently used in…

Computational Physics · Physics 2020-09-02 Eric J. Bylaska , Duo Song , Nicholas P. Bauman , Karol Kowalski , Daniel Claudino , Travis S. Humble

Core-level spectra of 1s electrons of elements heavier than Ne show significant relativistic effects. We combine advances in orbital optimized DFT (OO-DFT) with the spin-free exact two-component (X2C) model for scalar relativistic effects,…

Chemical Physics · Physics 2022-04-19 Leonardo A. Cunha , Diptarka Hait , Richard Kang , Yuezhi Mao , Martin Head-Gordon

We have developed a new basis set family, denoted aug-cc-pVnZ-F12 (or aVnZ-F12 for short), for explicitly correlated calculations. The sets included in this family were constructed by supplementing the corresponding cc-pVnZ-F12 sets with…

Chemical Physics · Physics 2017-12-27 Nitai Sylvetsky , Manoj Kumar Kesharwani , Jan M. L. Martin

Quantum phase estimation (QPE) is a promising quantum algorithm for obtaining molecular ground-state energies with chemical accuracy. However, its computational cost, dominated by the Hamiltonian 1-norm $\lambda$ and the cost of the block…

The perovskite oxides are known to be susceptible to structural distortions over a long wavelength when compared to their parent cubic structures. From an ab initio simulation perspective, this requires accurate calculations including many…

Computational Physics · Physics 2022-02-16 Jack S. Baker , Tsuyoshi Miyazki , David R. Bowler

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

We construct a reference benchmark set for atomic and molecular random-phase-approximation (RPA) correlation energies in a density functional theory (DFT) framework at the complete basis set limit. This set is used to evaluate the accuracy…

Chemical Physics · Physics 2013-02-22 E. Fabiano , F. Della Sala

We discuss, simplify, and improve the spin-dependent correction of L.A. Constantin et al., Phys. Rev. B 84, 233103, for atomization energies, and develop a density parameter of the form $v\propto |\nabla n|/n^{10/9}$, found from the…

Chemical Physics · Physics 2013-02-01 L. A. Constantin , E. Fabiano , F. Della Sala

Electronic structure methods for accurate calculation of molecular properties have a high cost that grows steeply with the problem size, therefore, it is helpful to have the underlying atomic basis functions that are less in number but of…

Chemical Physics · Physics 2019-03-15 Dimitri N. Laikov

Very recently, we introduced a set of correlation consistent effective core potentials (ccECPs) constructed within full many-body approaches. By employing significantly more accurate correlated approaches we were able to reach a new level…

Materials Science · Physics 2020-02-25 Abdulgani Annaberdiyev , Cody A. Melton , M. Chandler Bennett , Guangming Wang , Lubos Mitas

Knowledge of the repulsive behavior of potential energy curves $V(R)$ at $R\to0$ is necessary for understanding and modeling irradiation processes of practical interest. $V(R)$ is in principle straightforward to obtain from electronic…

Computational Physics · Physics 2020-03-09 Susi Lehtola

We demonstrate how to determine numerically nearly exact orthonormal orbitals that are optimal for evaluation of the energy of arbitrary (correlated) states of atoms and molecules by minimization of the energy Lagrangian. Orbitals are…

The method of increments and frozen natural orbital (MI-FNO) framework is introduced to help expedite the application of noisy, intermediate-scale quantum~(NISQ) devices for quantum chemistry simulations. The MI-FNO framework provides a…

We explore a separable resolution-of-the-identity formalism built on quadratures over limited sets of real-space points designed for all-electron calculations. Our implementation preserves in particular the use of common atomic orbitals and…

Chemical Physics · Physics 2019-05-22 Ivan Duchemin , Xavier Blase