Related papers: Complexity Reduction in Large Quantum Systems: Rel…

An accurate description of strong correlation is quintessential for the exploration of emerging chemical phenomena. While near-term variational quantum algorithms provide a theoretically scalable framework for quantum chemical problems, the…

Quantum-mechanically-driven charge polarization and charge transfer are ubiquitous in biomolecular systems, controlling reaction rates, allosteric interactions, ligand-protein binding, membrane transport, and dynamically-driven structural…

Hybrid quantum mechanics / molecular mechanics (QM/MM) models successfully describe the properties of biological macromolecules. However, most QM/MM methodologies are constrained to unrealistic gas phase models, thus limiting their…

Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…

We present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks orbitals, we assign an ad hoc electron…

Quantum embedding is an appealing route to fragment a large interacting quantum system into several smaller auxiliary `cluster' problems to exploit the locality of the correlated physics. In this work we critically review approaches to…

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Discretizing an analytic function on a uniform real-space grid is often done via a straightforward collocation method. This is ubiquitous in all areas of computational physics and quantum chemistry. An example in Density Functional Theory…

Recent advances in continuum embedding models have enabled the incorporation of solvent and electrolyte effects into density functional theory (DFT) simulations of material surfaces, significantly benefiting electrochemistry, catalysis, and…

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…

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…

Electronic polarization and dispersion are decisive actors in determining interaction energies between molecules. These interactions have a particularly profound effect on excitation energies of molecules in complex environments, especially…

We extend molecular bootstrap embedding to make it appropriate for implementation on a quantum computer. This enables solution of the electronic structure problem of a large molecule as an optimization problem for a composite Lagrangian…

Quantum computers (QC) could harbor the potential to significantly advance materials simulations, particularly at the atomistic scale involving strongly correlated fermionic systems where an accurate description of quantum many-body effects…

The stochastic density functional theory (DFT) [Phys. Rev. Lett. 111, 106402 (2013)] is a valuable linear scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is…

Quantum embedding theories are promising approaches to investigate strongly-correlated electronic states of active regions of large-scale molecular or condensed systems. Notable examples are spin defects in semiconductors and insulators. We…

Quantum effects of plasmonic phenomena have been explored through ab-initio studies, but only for exceedingly small metallic nanostructures, leaving most experimentally relevant structures too large to handle. We propose instead an…

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

This chapter presents controlled approximations of Kohn-Sham density functional theory (DFT) that enable very large scale simulations. The work is motivated by the study of defects in crystalline solids, though the ideas can be used in…

In a recent paper we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions is optimized in situ and therefore adapted to the chemical…