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We present a self consistent field approach (SCF) within the Adaptive Derivative-Assembled Problem-Tailored Ansatz Variational Quantum Eigensolver (ADAPT-VQE) framework for efficient quantum simulations of chemical systems on near-term…
Kohn-Sham Density Functional Theory (KS-DFT) has been traditionally solved by the Self-Consistent Field (SCF) method. Behind the SCF loop is the physics intuition of solving a system of non-interactive single-electron wave functions under…
We develop a stochastic formulation of the optimally-tuned range-separated hybrid density functional theory which enables significant reduction of the computational effort and scaling of the non-local exchange operator at the price of…
The sensitivity of computed DFT (Density Functional Theory) molecular properties (including energetics, geometries, vibrational frequencies, and infrared intensities) to the radial and angular numerical integration grid meshes, as well as…
The direct variational optimization of the two-electron reduced density matrix (2RDM) can provide a reference-independent description of the electronic structure of many-electron systems that naturally captures strong or nondynamic…
Multireference systems are usually challenging to investigate using ab initio methods as they require an accurate description of static electron correlation. The urgency of developing similar approaches is even more pressing when molecules…
The accurate description of the non-linear response of many-electron systems to strong-laser fields remains a major challenge. Methods that bypass the unfavorable exponential scaling with particle number are required to address larger…
A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…
The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD…
Projection-based embedding provides a simple, robust, and accurate approach for describing a small part of a chemical system at the level of a correlated wavefunction method while the remainder of the system is described at the level of…
Molecular ground-state simulation is one of the most promising fields for demonstrating practical quantum advantage on near-term quantum computers. However, the Variational Quantum Eigensolver (VQE), a leading algorithm for this task, still…
Reduced density-matrix functional theory (RDMFT) provides a variational route to electronic correlations beyond conventional density-functional approximations, but explicit evaluations of density-matrix functionals still scale exponentially…
The study of isolated defects in solids is a natural target for classical or quantum embedding methods that treat the defect at a high level of theory and the rest of the solid at a lower level of theory. Here, in the context of…
We present an accurate, efficient and massively parallel finite-element code, DFT-FE, for large-scale ab-initio calculations (reaching $\sim 100,000$ electrons) using Kohn-Sham density functional theory (DFT). DFT-FE is based on a local…
Minimizing the energy of an $N$-electron system as a functional of a two-electron reduced density matrix (2-RDM), constrained by necessary $N$-representability conditions (conditions for the 2-RDM to represent an ensemble $N$-electron…
We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…
A multiconfigurational adiabatic connection (AC) formalism is an attractive approach to computing dynamic correlation within CASSCF and DMRG models. Practical realizations of AC have been based on two approximations: i) fixing one- and…
The alignment of the frontier orbital energies of an adsorbed molecule with the substrate Fermi level at metal-organic interfaces is a fundamental observable of significant practical importance in nanoscience and beyond. Typical density…
Quantum algorithms for molecular electronic structure have been developed with lower computational scaling than their classical counterparts, but emerging quantum hardware is far from being capable of the coherence,connectivity and gate…
Density functional theory (DFT) is an efficient instrument for describing a wide range of nanoscale phenomena: wetting transition, capillary condensation, adsorption, etc. In this paper, we suggest a method for obtaining the equilibrium…