Related papers: The orbital minimization method for electronic str…
Given a set of Kohn-Sham orbitals from an insulating system, we present a simple, robust, efficient and highly parallelizable method to construct a set of, optionally orthogonal, localized basis functions for the associated subspace. Our…
We present a novel algorithm which can overcome the drawbacks of the conventional linear scaling method with minimal computational overhead. This is achieved by introducing additional constraints, thus eliminating the redundancy of the…
Spectral decomposition of linear operators plays a central role in many areas of machine learning and scientific computing. Recent work has explored training neural networks to approximate eigenfunctions of such operators, enabling scalable…
We propose a quantum-classical hybrid variational algorithm, the quantum orbital minimization method (qOMM), for obtaining the ground state and low-lying excited states of a Hermitian operator. Given parameterized ansatz circuits…
Within the framework of linear-scaling Kohn-Sham density functional theory, a robust method for maintaining compact localized orbitals close to the ground state is coupled with nuclear dynamics. This allows to obviate the commonly employed…
We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…
We present a method for total energy minimizations and molecular dynamics simulations based either on tight-binding or on Kohn-Sham hamiltonians. The method leads to an algorithm whose computational cost scales linearly with the system…
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…
The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…
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…
Near-term quantum computers will be limited in the number of qubits on which they can process information as well as the depth of the circuits that they can coherently carry out. To-date, experimental demonstrations of algorithms such as…
A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…
We present a code modularization approach to design efficient and massively parallel cubic and linear-scaling solvers for electronic structure calculations using atomic orbitals. The modular implementation of the orbital minimization…
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…
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…
Molecular dynamics simulations are indispensable for exploring the behavior of atoms and molecules. Grounded in quantum mechanical principles, quantum molecular dynamics provides high predictive power but its computational cost is dominated…
We present a method to discretize the Kohn-Sham Hamiltonian matrix in the pseudopotential framework by a small set of basis functions automatically contracted from a uniform basis set such as planewaves. Each basis function is localized…
We propose a state-averaged orbital optimization scheme for improving the accuracy of excited states of the electronic structure Hamiltonian for use on near-term quantum computers. Instead of parameterizing the orbital rotation operator in…
To obtain convergent numerical approximations without using any orthogonalization operations is of great importance in electronic structure calculations. In this paper, we propose and analyze a class of iteration schemes for the discretized…
In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…