Related papers: Efficient implementation of the superposition of a…
Repeated computations on the same molecular system, but with different geometries, are often performed in quantum chemistry, for instance, in ab-initio molecular dynamics simulations or geometry optimizations. While many efficient…
We introduce highly local basis sets for electronic structure which are very efficient for correlation calculations near the complete basis set limit. Our approach is based on gausslets, recently introduced wavelet-like smooth orthogonal…
We present an efficient \textit{ab initio} method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to…
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…
First principles calculations based on density functional theory are having an incerasing impact on our understanding of molecule-surface interactions. For example, calculations of the multi-dimensional potential energy surface have…
We have developed an efficient computational scheme utilizing the real-space finite-difference formalism and the projector augmented-wave (PAW) method to perform precise first-principles electronic-structure simulations based on the density…
In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…
The Gaussian Effective Potential (GEP) is shown to be a useful variational tool for the study of the magnetic properties of strongly correlated electronic systems. The GEP is derived for a single band Hubbard model on a two-dimensional…
We propose a simple scheme to construct composition-dependent interatomic potentials for multicomponent systems that when superposed onto the potentials for the pure elements can reproduce not only the heat of mixing of the solid solution…
The efficient computation of observables beyond the total energy is a key challenge and opportunity for fault-tolerant quantum computing approaches in quantum chemistry. Here we consider the symmetry-adapted perturbation theory (SAPT)…
We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…
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…
The central approximation made in classical molecular dynamics simulation of materials is the interatomic potential used to calculate the forces on the atoms. Great effort and ingenuity is required to construct viable functional forms and…
We present a computationally efficient approach to perform large-scale all-electron density functional theory calculations by enriching the classical finite element basis with compactly supported atom-centered numerical basis functions that…
Physically-motivated and mathematically robust atom-centred representations of molecular structures are key to the success of modern atomistic machine learning (ML) methods. They lie at the foundation of a wide range of methods to predict…
Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…
We show that the Gaussian Approximation Potential machine learning framework can describe complex magnetic potential energy surfaces, taking ferromagnetic iron as a paradigmatic challenging case. The training database includes total…
Electronic susceptibilities are a very popular tool to study electronic and magnetic properties of materials, both in experiment and theory. Unfortunately, the numerical evaluation of even the bare susceptibility, which depends on the…
We present a new density-functional method of the self-consistent electronic-structure calculation which does not exploit any local density approximations (LDA). We use the exchange-correlation energy which consists of the exact exchange…
As the first component of SPARC (Simulation Package for Ab-initio Real-space Calculations), we present an accurate and efficient finite-difference formulation and parallel implementation of Density Functional Theory (DFT) for isolated…