相关论文: Direct determination of optimal real-space orbital…

An energy functional for orbital based $O(N)$ calculations is proposed, which depends on a number of non orthogonal, localized orbitals larger than the number of occupied states in the system, and on a parameter, the electronic chemical…

The choice of molecular orbitals is decisive in configuration interaction calculations. In this letter, a democratic description of the ground and excited states follows an orthogonally constrained orbitals optimization to produce…

Rydberg excited states of molecules pose a challenge for electronic structure calculations because of their highly diffuse electron distribution. Even large and elaborate atomic basis sets tend to underrepresent the long-range tail, overly…

The need for accurate calculations on atoms and diatomic molecules is motivated by the opportunities and challenges of such studies. The most commonly-used approach for all-electron electronic structure calculations in general - the linear…

In electronic structure theory, variational methods offer a valuable paradigm for approximating electronic ground states. However, for historical reasons, this principle is mostly restricted to model chemistries in pre-defined fixed basis…

Variational quantum eigensolver ans\"atze hold considerable promise for ground-state energy calculations on near-term quantum hardware, yet most promising ansatz designs currently strongly depend on how well the molecular orbital basis…

In pursuit of a minimal basis for systems with non-ideal bond angles, in this work we try to pinpoint the exact orientation of the major overlapping orbitals along the nearest neighbouring coordination segments in a given system such that…

The accuracy of reaction energy profiles calculated with multi-configurational electronic structure methods and corrected by multi-reference perturbation theory depends crucially on consistent active orbital spaces selected along the…

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…

Complete orthonormal sets of exponential-type orbitals with non-integer principal quantum numbers are discussed as basis functions in non-relativistic Hartree-Fock-Roothaan electronic structure calculations of atoms. A method is proposed to…

Atomic orbitals underpin our understanding of electronic structure, providing intuitive descriptions of bonding, charge transfer, magnetism, and correlation effects. Despite their utility, an atomic basis that is adaptable, strictly…

The Hartree-Fock-Rothaan equations are solved for He-like ions using the iterative self-consistent method. New complete and orthonormal sets of exponential-type orbitals are employed as the basis. These orbitals satisfy the orthonormality…

In this paper, we propose a parallel optimization method for electronic structure calculations based on a single orbital-updating approximation. It is shown by our numerical experiments that the method is efficient and reliable for atomic…

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…

Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…

In this paper, we propose a generic and systematic approach for study of the electronic structure for atoms or molecules. In particular, we address the issue of single particle states, or orbitals, which should be one of the most important…

The implementation of the orbital minimization method (OMM) for solving the self-consistent Kohn-Sham (KS) problem for electronic structure calculations in a basis of non-orthogonal numerical atomic orbitals of finite-range is reported. We…

We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…

A method for increasing the accuracy of configuration interaction (CI) calculations of molecules and other electronic systems is proposed. The energy defect of a given calculation is associated with the electron pair origin of…

We propose simple analytic, non-orthogonal but selectively orthogonalizable, generalized Laguerre type atomic orbitals, providing clear physical interpretation and near equivalent accuracy with numerical multi-configuration self-consistent…