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One of the primary challenges in quantum chemistry is the accurate modeling of strong electron correlation. While multireference methods effectively capture such correlation, their steep scaling with system size prohibits their application…
Quantum simulations of metal surfaces are critical for catalytic innovation. Yet existing methods face a cost-accuracy dilemma: density functional theory is efficient but system-dependent in accuracy, while wavefunction-based theories are…
In transitions between different environmental settings, a molecular system inevitably undergoes a range of detectable changes, and the ability to accurately simulate such responses, e.g., in the form of shifts to molecular energies,…
We present an efficient computational approach to perform real-space electronic structure calculations using an adaptive higher-order finite-element discretization of Kohn-Sham density-functional theory (DFT). To this end, we develop an…
Localized representation of the Kohn-Sham subspace plays an important role in quantum chemistry and materials science. The recently developed selected columns of the density matrix (SCDM) method [J. Chem. Theory Comput. 11, 1463, 2015] is a…
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…
In this paper we develop a simple finite element method for simulation of embedded layers of high permeability in a matrix of lower permeability using a basic model of Darcy flow in embedded cracks. The cracks are allowed to cut through the…
We present an embedding scheme for periodic systems that facilitates the treatment of the physically important part (here the unit cell) with advanced electronic-structure methods, that are computationally too expensive for periodic…
An extended first-principles molecular dynamics (FPMD) method based on Kohn-Sham scheme is proposed to elevate the temperature limit of the FPMD method in the calculation of dense plasmas. The extended method treats the wave functions of…
In this work, we introduce an original self-consistent scheme based on the one-body reduced density matrix ($\gamma$) formalism. A significant feature of this methodology is the utilization of an optimal unitary transformation of the…
In complex systems, it is often the case that the region of interest forms only one part of a much larger system. The idea of joining two different quantum simulations - a high level calculation on the active region of interest, and a low…
To reduce the rapidly growing computational cost of the dual fermion lattice calculation with increasing system size, we introduce two embedding schemes. One is the real fermion embedding, and the other is the dual fermion embedding. Our…
Recent trends of ab initio studies and progress in methodologies for electronic structure calculations of strongly correlated electron systems are discussed. The interest for developing efficient methods is motivated by recent discoveries…
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…
We introduce a new approach to density functional theory based on kinetic theory, showing that the Kohn-Sham equations can be derived as a macroscopic limit of a suitable Boltzmann kinetic equation in the limit of small mean free path…
We propose to expand the territory of density functional theory to strongly correlated electrons by reformulating the Kohn-Sham scheme in the representation of fractionalized particles. We call it the ``KS* scheme.'' Using inhomogeneous…
Large scale atomistic simulations with suitable interatomic potentials are widely employed by scientists or engineers of different areas. Quick generation of high-quality interatomic potentials is of urgent need under present circumstances,…
We present an approach to solid-state electronic-structure calculations based on the finite-element method. In this method, the basis functions are strictly local, piecewise polynomials. Because the basis is composed of polynomials, the…
A new repeated-slab calculation method is developed to simulate the electronic structures of charged surfaces by arranging density-variable charged sheets in vacuum regions to realize a constant potential on the charged sheets and maintain…
In this work we give a comprehensive derivation of an exact and numerically feasible method to perform ab-initio calculations of quantum particles interacting with a quantized electromagnetic field. We present a hierachy of…