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The simulation of molecular electronic structure is an important application of quantum devices. Recently, it has been shown that quantum devices can be effectively combined with classical supercomputing centers in the context of the…
Reliable and robust convergence to the electronic ground state within density functional theory (DFT) Kohn-Sham (KS) calculations remains a thorny issue in many systems of interest. In such cases, charge sloshing can delay or completely…
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…
The computation of excited electronic states is an important application for quantum computers. In this work, we simulate the excited state spectra of four aromatic heterocycles on IBM superconducting quantum computers, focusing on active…
We present an accurate and efficient formulation of the stress tensor for real-space Kohn-Sham Density Functional Theory (DFT) calculations. Specifically, while employing a local formulation of the electrostatics, we derive a linear-scaling…
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) allows for predicting all the chemical and physical properties of molecular systems from first principles by finding an approximate solution to the many-body Schr\"odinger equation. However, the cost of these…
We applied renormalized singles (RS) in the multireference density functional theory (DFT) to calculate accurate energies of ground and excited states. The multireference DFT approach determines the total energy of the $N$-electron system…
Improving the predictive capability of molecular properties in ab initio simulations is essential for advanced material discovery. Despite recent progress making use of machine learning, utilizing deep neural networks to improve quantum…
Excited states of molecules lie in the heart of photochemistry and chemical reactions. The recent development in quantum computational chemistry leads to inventions of a variety of algorithms that calculate the excited states of molecules…
Efficient molecular dynamics (MD) simulation is vital for understanding atomic-scale processes in materials science and biophysics. Traditional density functional theory (DFT) methods are computationally expensive, which limits the…
The nuclear-electronic orbital (NEO) method is a well-established approach for treating nuclei quantum mechanically in molecular systems beyond the usual Born-Oppenheimer approximation. In this work, we present a strategy to implement the…
Density functional theory (DFT) serves as the basis for computational discovery in materials science and chemistry, yet each calculation demands extensive human effort: adjusting algorithms when convergence stalls, revising plans when…
Quantum-mechanical simulations can offer atomic-level insights into chemical processes on surfaces. This understanding is crucial for the rational design of new solid catalysts as well as materials to store energy and mitigate greenhouse…
The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…
A Kohn-Sham density-functional energy expression is derived for any (ground or excited) state within a given many-electron ensemble along with the stationarity condition it fulfills with respect to the ensemble density, thus giving access…
The present work demonstrates a robust protocol for probing localized electronic structure in condensed-phase systems, operating in terms of a recently proposed theory for decomposing the results of Kohn-Sham density functional theory in a…
We present a tensor-structured algorithm for efficient large-scale DFT calculations by constructing a Tucker tensor basis that is adapted to the Kohn-Sham Hamiltonian and localized in real-space. The proposed approach uses an additive…
To overcome the limitations of the traditional state-averaging approaches in excited state calculations, where one solves for and represents all states between the ground state and excited state of interest, we have investigated a number of…
The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…