相关论文: Molecule-optimized Basis Sets and Hamiltonians for…

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…

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…

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…

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…

Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many…

We investigate the use of optimized correlation consistent gaussian basis sets for the study of insulating solids with auxiliary-field quantum Monte Carlo (AFQMC). The exponents of the basis set are optimized through the minimization of the…

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 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…

Multicomponent methods are a conceptually simple way to include nuclear quantum effects into quantum chemistry calculations. In multicomponent methods, the electronic molecular orbitals are described using the linear combination of atomic…

Most modern calculations of many-electron atoms use basis sets of atomic orbitals. An accurate account for the electronic correlations in heavy atoms is very difficult computational problem and optimization of the basis sets can reduce…

A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…

Electronic structure calculations on small systems such as H$_2$, H$_2$O, LiH, and BeH$_2$ with chemical accuracy are still a challenge for the current generation of the noisy intermediate-scale quantum (NISQ) devices. One of the reasons is…

We investigate the basis-set convergence of electronic correlation energies calculated using coupled cluster theory and a recently proposed finite basis-set correction technique. The correction is applied to atomic and molecular systems and…

We have recently discussed an algorithm to automatically generate auxiliary basis sets (ABSs) of the standard form for density fitting (DF) or resolution-of-the-identity (RI) calculations in a given atomic orbital basis set (OBS) of any…

Density fitting (DF), also known as the resolution of the identity (RI), is a widely used technique in quantum chemical calculations with various types of atomic basis sets - Gaussian-type orbitals, Slater-type orbitals, as well as…

The performance of basis sets made of numerical atomic orbitals is explored in density-functional calculations of solids and molecules. With the aim of optimizing basis quality while maintaining strict localization of the orbitals, as…

We present a fully numerical framework for the optimization of molecule-specific quantum chemical basis functions within the quantics tensor train format using a finite-difference scheme. The optimization is driven by solving the…

With the recent advances in the development of devices capable of performing quantum computations, a growing interest in finding near-term applications has emerged in many areas of science. In the era of non-fault tolerant quantum devices,…

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…

In this contribution, we employ a density matrix based optimization procedure to obtain customized basis functions to describe chains of rotating water molecules in interaction regimes associated with different intermolecular distances.…