Related papers: Developing correlation-consistent numeric atom-cen…
An attractive way to model nuclear quantum effects is to describe select nuclei quantum mechanically at the same level as the electrons. This non-Born-Oppenheimer (non-BO) method is known by many names including the nuclear-electronic…
We present an all-electron, periodic {\GnWn} implementation within the numerical atomic orbital (NAO) basis framework. A localized variant of the resolution-of-the-identity (RI) approximation is employed to significantly reduce the…
We aim to develop novel reusable open source infrastructure [Lehtola, J. Chem. Phys. 159, 180901 (2023)] for numerical atomic orbitals (NAOs). Soft confinement potentials are typically used to force the NAO radial basis functions…
Relativistic quintuple-zeta basis sets for the p elements are presented. The basis sets for the occupied spinors were optimized at the Dirac-Coulomb self-consistent field (SCF) level on the ground configurations. Valence and core…
As an extension to our previous work [1], a comprehensive theoretical study for Na-like Krypton and Xenon is carried out. Using MCDHF (Multiconfiguration Dirac-Hartee-Fock) along with RDW (Relativistic distorted wave) theory we calculate…
The nuclear-electronic orbital (NEO) method is a well-established approach for treating nuclei quantum mechanically in molecular systems beyond the usual Born-Oppenheimer approximation. In this work, we present a strategy to implement the…
Ab initio calculations face the challenge of describing a complex multiscale quantum many-body system. The nuclear wave function has both strong short-range correlations and long-range contributions. Natural orbitals provide a means of…
We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold…
The cost of simulating quantum many-body systems - on classical or quantum hardware - scales with the number of variational parameters, so progress at fixed computational budget hinges on more parameter-efficient ans\"atze. Configuration…
Density functional theory with plane-wave basis sets is widely employed in computational materials science, including applications to isolated molecular systems. However, the inadequate description of electron correlation remains a…
The random phase approximation (RPA) for the correlation energy functional of density functional theory has recently attracted renewed interest. Formulated in terms of the Kohn-Sham (KS) orbitals and eigenvalues, it promises to resolve some…
Atomic basis sets are widely employed within quantum mechanics based simulations of matter. We introduce a machine learning model that adapts the basis set to the local chemical environment of each atom, prior to the start of self…
We introduce a method for solving a self consistent electronic calculation within localized atomic orbitals, that allows us to converge to the complete basis set (CBS) limit in a stable, controlled, and systematic way. We compare our…
Variational quantum eigensolvers (VQE) are among the most promising approaches for solving electronic structure problems on near-term quantum computers. A critical challenge for VQE in practice is that one needs to strike a balance between…
In non-self-consistent calculations of the total energy within the random-phase approximation (RPA) for electronic correlation, it is necessary to choose a single-particle Hamiltonian whose solutions are used to construct the electronic…
We present a formulation and implementation of the DFT+\textit{U} method within the framework of linear combination of numerical atomic orbitals (NAO). Our implementation not only enables single-point total energy and electronic-structure…
Reliable computational methodologies and basis sets for modeling x-ray spectra are essential for extracting and interpreting electronic and structural information from experimental x-ray spectra. In particular, the trade-off between…
Nuclear quantum effects such as zero-point energy and hydrogen tunnelling play a central role in many biological and chemical processes. The nuclear-electronic orbital (NEO) approach captures these effects by treating selected nuclei…
A new approach to approximate the kinetic-energy-functional dependent component ($v_t[\rho_A,\rho_B](\vec{r})$) of the effective potential in one-electron equations for orbitals embedded in a frozen density environment (Eqs. 20-21 in…
The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis…