Related papers: Accurate ionic forces and geometry optimisation in…
Accurate and efficient theoretical techniques for describing ionic fluids are highly desirable for many applications across the physical, biological and materials sciences. With a rigorous statistical mechanical foundation, classical…
We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…
We introduce a method for computing quantum mechanical forces through surface integrals over the stress tensor within the framework of density functional theory. This approach avoids the inaccuracies of traditional force calculations using…
Approximate semi-local density functional theory (DFT) is known to underestimate surface formation energies yet paradoxically overbind adsorbates on catalytic transition-metal oxide surfaces due to delocalization error. The low-cost DFT+U…
Density-functional theory (DFT) has revolutionized computer simulations in chemistry and material science. A faithful implementation of the theory requires self-consistent calculations. However, this effort involves repeatedly diagonalizing…
Density functional theory (DFT) is an indispensable ab initio method in both quantum chemistry and condensed matter physics. Based on recent advancements in reduced density matrix functional theory (RDMFT), a variant of DFT that is believed…
Developing reliable pseudopotentials for orbital-free density functional theory (OF-DFT), especially for transition metals, remains a significant challenge. In this study, we provide a theoretical framework for analyzing pseudization…
Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…
We show that the energetics and lifetimes of resonances of finite systems under an external electric field can be captured by Kohn--Sham density functional theory (DFT) within the formalism of uniform complex scaling. Properties of…
We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…
In the exact Kohn-Sham density-functional theory (DFT), the total energy versus the number of electrons is a series of linear segments between integer points. However, commonly used approximate density functionals produce total energies…
In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…
Density Functional Theory calculations traditionally suffer from an inherent cubic scaling with respect to the size of the system, making big calculations extremely expensive. This cubic scaling can be avoided by the use of so-called linear…
First-principles density functional theory (DFT) codes which employ a localized basis offer advantages over those which use plane-wave bases, such as better scaling with system size and better suitability to low-dimensional systems. The…
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 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 to perform fully selfconsistent density-functional calculations, which scales linearly with the system size and which is well suited for very large systems. It uses strictly localized pseudoatomic orbitals as basis…
We present the first mathematical analysis of stochastic density functional theory (DFT) in the context of the Hartree approximation. We motivate our analysis via the notion of nearly-optimal or $\tilde{O}(n)$ scaling with respect to the…
We present a method to make highly accurate pseudopotentials for use with orbital-free density functional theory (OF-DFT) with given exchange-correlation and kinetic energy functionals, which avoids the compounding of errors of Kohn-Sham…
Recently, we have proposed the adaptive local basis set for electronic structure calculations based on Kohn-Sham density functional theory in a pseudopotential framework. The adaptive local basis set is efficient and systematically…