Related papers: Natural-orbital representation of molecular electr…
Transport in molecular electronic devices is different from that in semiconductor mesoscopic devices in two important aspects: (1) the effect of the electronic structure and (2) the effect of the interface to the external contact. A…
The last several decades have seen significant advances in the theoretical modeling of materials within the fields of solid-state physics and materials science, but many methods commonly applied to this problem struggle to capture strong…
Methods for electronic structure based on Gaussian and molecular orbital discretizations offer a well established, compact representation that forms much of the foundation of correlated quantum chemistry calculations on both classical and…
The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…
Occupation numbers of natural orbitals capture the physics of strong electron correlations in momentum space. A Natural Orbital Density Functional Theory based on the antisymmetrized geminal product provides these occupation numbers and the…
We investigate the suitability of natural orbitals as a basis for describing many-body excitations. We analyze to which extend the natural orbitals describe both bound as well as ionized excited states and show that depending on the…
This contribution reports the study of a set of molecular electronic-structure reorganization representations related to light-induced electronic transitions, modeled in the framework of time-dependent density-functional response theory.…
We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…
We present a reduced density operator for electronically open molecules by explicitly averaging over the environmental degrees of freedom of the composite Hamiltonian. Specifically, we include the particle-number non-conserving…
Natural orbitals, defined in electronic structure and quantum chemistry as the (molecular) orbitals diagonalizing the one-particle reduced density matrix of the ground state, have been conjectured for decades to be the perfect reference…
In the recent work of S. Sharma \emph{et al.}, (arxiv.org: arxiv:0912.1118), a single-electron spectrum associated with the natural orbitals was defined as the derivative of the total energy with respect to the occupation numbers at half…
The one-particle reduced density-matrix (1-RDM) functional theory is a promising alternative to density-functional theory (DFT) that uses the 1-RDM rather than the electronic density as a basic variable. However, long-standing challenges…
Using generalizations of natural orbitals, spin-averaged natural orbitals, and two-particle charge correlators for solids, we investigate electronic structure of antiferromagnetic transition-metal oxides with a fully self-consistent,…
An accurate expression of the kinetic energy density of an electronic distribution in terms of the single particle reduced density matrix for atomic and molecular systems is a long-standing problem in electron structure theory. Existing…
We introduce a novel energy functional for ground-state electronic-structure calculations. Its fundamental variables are the natural spin-orbitals of the implied singlet many-body wave function and their joint occupation probabilities. The…
We introduce the concept of natural super-orbitals for many-body operators, defined as the eigenvectors of the one-body super-density matrix associated with a vectorized operator. We relate these objects to measures of non-Gaussianity of…
The study of electronic transitions within a molecule connected to the absorption or emission of light is a common task in the process of the design of new materials. The transitions are complex quantum mechanical processes and a detailed…
A natural orbital functional for electronic systems with any value of the spin is proposed. This energy functional is based on a new reconstruction for the two-particle reduced density matrix (2RDM) of the multiplet, that is, of the mixed…
The analytic energy gradients in the atomic orbital representation have recently been published (J. Chem. Phys. 146, 014102, 2017) within the framework of the natural orbital functional theory (NOFT). We provide here an alternative…
We apply reduced density-matrix functional theory to the parabolically confined quantum Hall droplet in the spin-frozen strong magnetic field regime. One-body reduced density matrix functional method performs remarkably well in obtaining…