Related papers: Geminal embedding scheme for optimal atomic basis …
Neural-network quantum states offer a flexible route to compact many-electron wave functions, but their practical accuracy depends strongly on how fermionic antisymmetry, electron correlation, and optimization noise are treated. Here we…
We propose a unique scheme to construct fully optimized atomic basis sets for density-functional calculations. The shapes of the radial functions are optimized by minimizing the {\it spillage} of the wave functions between the atomic…
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…
We introduce a simple generalization of the well known geminal wavefunction already applied in Quantum Chemistry to atoms and small molecules. The main feature of the proposed wavefunction is the presence of the antisymmetric geminal part…
A simple scheme is described for introducing the correct cusps at nuclei into orbitals obtained from Gaussian basis set electronic structure calculations. The scheme is tested with all-electron variational quantum Monte Carlo (VMC) and…
We show the transformation from a one-particle basis to a geminal basis, transformations between different geminal bases and demonstrate the Lie algebra of a geminal basis. From the basis transformations we express both the wave function…
A simple yet general method for constructing basis sets for molecular electronic structure calculations is presented. These basis sets consist of atomic natural orbitals from a multi-configurational self-consistent field calculation…
In high magnetic field calculations, anisotropic Gaussian type orbital (AGTO) basis functions are capable of reconciling the competing demands of the spherically symmetric Coulombic interaction and cylindrical magnetic ($B$ field)…
We report a quantum Monte Carlo (QMC) study, on a very simple but nevertheless very instructive model system of four hydrogen atoms, recently proposed in Ref. 1. We find that the Jastrow correlated Antisymmetrized Geminal Power (JAGP) is…
Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…
Diradical molecules are essential species involved in many organic and inorganic chemical reactions. The computational study of their electronic structure is often challenging, because a reliable description of the correlation, and in…
We show that a simple correlated wave function, obtained by applying a Jastrow correlation term to an Antisymmetrized Geminal Power (AGP), based upon singlet pairs between electrons, is particularly suited for describing the electronic…
Herein, we report accurate atomization energy calculations for 55 molecules in the Gaussian-2 (G2) set using lattice regularized diffusion Monte Carlo (LRDMC). We compare the Jastrow-Slater determinant ansatz with a more flexible JsAGPs…
We present a new adaptive method for electronic structure calculations based on novel fast algorithms for reduction of multivariate mixtures. In our calculations, spatial orbitals are maintained as Gaussian mixtures whose terms are selected…
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 elaborate on unconventional electronic structure methods based on geminals and their potential to advance the rapidly developing field of organic photovoltaics (OPV). Specifically, we focus on the computational advantages of…
Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control…
We present a modification to variational Monte Carlo's linear method optimization scheme that addresses a critical memory bottleneck while maintaining compatibility with both the traditional ground state variational principle and our…
For variational algorithms on the near term quantum computing hardware, it is highly desirable to use very accurate ansatze with low implementation cost. Recent studies have shown that the antisymmetrized geminal power (AGP) wavefunction…
We extend the Coleman's antisymmetrized geminal power (AGP) to develop a wave function theory that can incorporate up to four-body correlation in a region of strong correlation. To facilitate the variational determination of the wave…