Related papers: Embedded-Cluster Calculations in a Numeric Atomic …
Quantum computers can be used to calculate the electronic structure and estimate the ground state energy of many-electron molecular systems. In the present study, we implement the Variational Quantum Eigensolver (VQE) algorithm, as a hybrid…
The basic idea of Frozen-Density Embedding Theory (FDET) is the constrained minimisation of the Hohenberg-Kohn density functional $E^{HK}[\rho]$ performed using the auxiliary functional $E_{v_{AB}}^{FDET}[\Psi_A,\rho_B]$, where $\Psi_A$ is…
Adiabatic mixed quantum/classical molecular dynamics simulations were used to generate snapshots of the hydrated electron (e-) in liquid water at 300 K. Water cluster anions that include two complete solvation shells centered on the e- were…
We present SPARC-atomSFE, a spectral finite-element package for accurate and efficient atomic structure calculations within the framework of Kohn-Sham density functional theory. The package supports both all-electron and norm conserving…
Given a partition of a large system into an active quantum mechanical (QM) region and its environment, we present a simple way of embedding the QM region into an effective electrostatic potential representing the environment. This potential…
Performing high accuracy hybrid functional calculations for condensed matter systems containing a large number of atoms is at present computationally very demanding - when not out of reach - if high quality basis sets are used. We present a…
Quantum embedding theories are promising approaches to investigate strongly-correlated electronic states of active regions of large-scale molecular or condensed systems. Notable examples are spin defects in semiconductors and insulators. We…
Accurately modeling the electronic structure of materials is a persistent challenge to high-throughput screening. A promising means of balancing accuracy against computational cost are non-self-consistent calculations with hybrid…
Million-atom quantum simulations are in principle feasible with Orbital-Free Density Functional Theory (OF-DFT) because the algorithms only require simple functional minimizations with respect to the electron density function. In this…
Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. An efficient algorithm for the…
Chemical accuracy serves as an important metric for assessing the effectiveness of the numerical method in Kohn--Sham density functional theory. It is found that to achieve chemical accuracy, not only the Kohn--Sham wavefunctions but also…
We present a spectral scheme for atomic structure calculations in pseudopotential Kohn-Sham density functional theory. In particular, after applying an exponential transformation of the radial coordinates, we employ global polynomial…
A cardinal obstacle to performing quantum-mechanical simulations of strongly-correlated matter is that, with the theoretical tools presently available, sufficiently-accurate computations are often too expensive to be ever feasible. Here we…
We outline a strategy to compute deeply inelastic scattering structure functions using a hybrid quantum computer. Our approach takes advantage of the representation of the fermion determinant in the QCD path integral as a quantum mechanical…
The interaction between electronic and nuclear spins in the presence of external magnetic fields can be described by a spin Hamiltonian, with parameters obtained from first principles, electronic structure calculations. We describe an…
In common with many high-accuracy electronic structure methods, the initiator adaptation of full configuration interaction quantum Monte Carlo (i-FCIQMC) has difficulty treating realistic systems with large numbers of electrons. This…
Molecular motion at metallic surfaces is affected by nonadiabatic effects and electron-phonon coupling. The ensuing energy dissipation and dynamical steering effects are not captured by classical molecular dynamics simulations, but can be…
Nonlocal kinetic energy density functionals (KEDFs) with density-dependent kernels are currently the most accurate functionals available for orbital-free density functional theory (OF-DFT) calculations. However, despite advances in…
Quantum computers hold promise to improve the efficiency of quantum simulations of materials and to enable the investigation of systems and properties more complex than tractable at present on classical architectures. Here, we discuss…
This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…