Related papers: Electronic Transitions for a Fully Polarizable QM/…
Polarizable Quantum Mechanics/Molecular Mechanics (QM/MM) approaches based on fluctuating charges and dipoles (QM/FQ(F$\mu$)) are formulated within the state-specific Vertical Excitation Model (VEM) to compute vertical excitation energies…
The fully polarizable QM/MM approach based on fluctuating charges and fluctuating dipoles, named QM/FQF{\mu} (J. Chem. Theory Comput. 2019, 15, 2233-2245), is extended to the evaluation of nuclear gradients and the calculation of IR spectra…
A multiscale model based on the coupling of the multiconfigurational self-consistent field (MCSCF) method and the classical atomistic polarizable Fluctuating Charges (FQ) force field is presented. The resulting MCSCF/FQ approach is…
We present a computational study of static and dynamic linear polarizabilities in solution. We use different theoretical approaches to describe solvent effects, ranging from quantum mechanics/molecular mechanics (QM/MM) to quantum embedding…
We present the extension of the quantum/classical polarizable fluctuating charge model to the calculation of single residues of quadratic response functions, as required for the computational modeling of two-photon absorption…
Fluctuating-charge models are computationally efficient methods of treating polarization and charge-transfer phenomena in molecular mechanics and classical molecular dynamics simulations. They are also theoretically appealing as they are…
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…
Treating water as a linearly responding dielectric continuum on molecular length scales allows very simple estimates of solvation structure and thermodynamics for charged and polar solutes. While this approach can successfully account for…
Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…
Fluctuating-charge models have been used to model polarization effects in molecular mechanics methods. However, they overestimate polarizabilities in large systems. Previous attempts to remedy this have been at the expense of forbidding…
The performance of different Quantum Mechanics/Molecular Mechanics embedding models to compute vacuo-to-water solvatochromic shifts are investigated. In particular, both non-polarizable and polarizable approaches are analyzed and computed…
Polaron-transformed quantum master equation (PQME) offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of freedom. Thus, PQME serves as an efficient…
We present an extension of the standard polarizable quantum mechanic/molecular mechanics (QM/MM) approach for treating environmental effects on excited state properties of embedded systems. A quantum polarizable atom model is derived from a…
We present a novel hybrid quantum/classical (QM/MM) approach to the calculation of charged excitations in molecular solids based on the many-body Green's function $GW$ formalism. Molecules described at the $GW$ level are embedded into the…
A new molecular dynamics model in which the point charges on atomic sites are allowed to fluctuate in response to the environment is developed and applied to water. The idea for treating charges as variables is based on the concept of…
We present a general computational protocol for the evaluation of extensive molecular response properties in complex environments within a polarizable quantum embedding framework. The approach extends multilevel density functional theory…
Our previously introduced QTPIE (charge transfer with polarization current equilibration) model (J. Chen and T. J. Martinez, Chem. Phys. Lett. 438, 315 (2007)) is a fluctuating-charge model with correct asymptotic behavior. Unlike most…
Classical molecular dynamics simulations have recently become a standard tool for the study of electrochemical systems. State-of-the-art approaches represent the electrodes as perfect conductors, modelling their responses to the charge…
Quantum Monte Carlo (QMC) is a stochastic method which has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that, within a…
The potential of mean-field decomposition techniques in interpreting electronic transitions in molecules is explored, particularly, the usefulness of these for offering computational signatures of different classes of such excitations. When…