Related papers: A polarizable CASSCF/MM approach using the interfa…
The structure and function of biological molecules are strongly influenced by the water and dissolved ions that surround them. This aqueous solution (solvent) exerts significant electrostatic forces in response to the biomolecule's…
Including the effect of the molecular environment in the numerical modeling of time-resolved electronic spectroscopy remains an important challenge in computational spectroscopy. In this contribution, we present a general approach for the…
We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis, and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with system…
We present a many-body $GW$ formalism for quantum subsystems embedded in discrete polarizable environments containing up to several hundred thousand atoms described at a fully ab initio random phase approximation level. Our approach is…
Machine learning and specifically deep-learning methods have outperformed human capabilities in many pattern recognition and data processing problems, in game playing, and now also play an increasingly important role in scientific…
We present a generalization of the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method to cavity quantum-electrodynamical (QED) matter systems. The method can be formulated in both the Coulomb and the dipole gauge. We verify its…
Accurate modeling of surface catalytic processes often requires methods capable of describing strong correlation, charge transfer, and multiple closely lying electronic states. While density functional theory remains widely used, its…
Near-term quantum computers are expected to facilitate material and chemical research through accurate molecular simulations. Several developments have already shown that accurate ground-state energies for small molecules can be evaluated…
Combinatorial materials libraries are an efficient route to generate large families of candidate compositions, but their impact is often limited by the speed and depth of characterization and by the difficulty of extracting actionable…
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…
We review recent advances in the capabilities of the open source ab initio Quantum Monte Carlo (QMC) package QMCPACK and the workflow tool Nexus used for greater efficiency and reproducibility. The auxiliary field QMC (AFQMC) implementation…
The scalar mode polarization of the cosmic microwave background is derived in a spatially closed universe from the Boltzmann equation using the line of sight integral method. The EE and TE multipole coefficients have been extracted…
The accuracy and efficiency of a coarse-grained (CG) force field are pivotal for high-precision molecular simulations of large systems with complex molecules. We present an automated mapping and optimization framework for molecular…
QM/MM hybrid methods employ accurate quantum (QM) models only in regions of interest (defects) and switch to computationally cheaper interatomic potential (MM) models to describe the crystalline bulk. We develop two QM/MM hybrid methods for…
OPENMMF is a numerical library designed to evaluate the Time-Evolution Operator of quantum systems with a discrete spectrum, and driven by an arbitrary combination of harmonic couplings. The time-evolution operator is calculated as a…
Biomolecular thermodynamics and spectroscopy depend on relative conformer energies, local curvatures, and collective dipole fluctuations on the potential-energy surface. Conventional molecular mechanics force fields enable large-scale…
Electrochemical processes play a crucial role in energy storage and conversion systems, yet their computational modeling remains a significant challenge. Accurately incorporating the effects of electric potential has been a central focus in…
Spin-orbit coupling (SOC) is incorporated into the phaseless plane-wave-based auxiliary-field quantum Monte Carlo (pw-AFQMC) method. This integration is implemented using optimized multiple-projector norm-conserving pseudopotentials, which…
Simulations of colloidal suspensions consisting of mesoscopic particles and smaller species such as ions or depletants are computationally challenging as different length and time scales are involved. Here, we introduce a machine learning…
Predicting the adsorption affinity of a small molecule to a target surface is of importance to a range of fields, from catalysis to drug delivery and human safety, but a complex task to perform computationally when taking into account the…