化学物理
To expand the existing QUEST database of accurate vertical transition energies [\href{https://doi.org/10.1002/wcms.1517}{V\'eril et al.~\textit{WIREs Comput.~Mol.~Sci.} \textbf{2021}, \textit{11}, e1517}], we have modeled more than 100…
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…
We prove both analytically and numerically that the total angular momentum of a molecular system undergoing adiabatic Born-Oppenheimer dynamics is conserved only when pseudo-magnetic Berry forces are taken into account. This finding sheds…
We propose a framework for describing the dynamics associated with the adsorption of small molecules to liquid-vapor interfaces, using an intermediate resolution between traditional continuum theories that are bereft of molecular detail and…
In this work, a force field for several ions in water is proposed. In particular, we consider the cations Li$^+$ , Na$^+$ , K$^+$, Mg$^{2+}$, Ca$^{2+}$ and the anions Cl$^-$, and SO$_4^{2-}$ . These ions were selected as they appear in the…
Many important processes affecting the Earth's climate are determined by the physical properties of seawater. Desalination of seawater is a significant source of drinking wate.Since the physical properties of seawater governing these…
In this work, we have computed electrical conductivities at ambient conditions of aqueous NaCl and KCl solutions by using the Einstein-Helfand equation. Common force fields (charge q = 1 e) do not reproduce the experimental values of…
Ice nucleation is a phenomenon that, despite the relevant implications for life, atmospheric sciences, and technological applications, is far from being completely understood, especially under extreme thermodynamic conditions. In this work…
Accurate predictions for hydrogen molecular levels require the treatment of electrons and nuclei on an equal footing. While nonrelativistic theory has been effectively formulated this way, calculation of relativistic and quantum…
We present a complete calculation, fully accounting for quantum effects and for molecular flexibility, of the first dielectric virial coefficient of water and its isotopologues. The contribution of the electronic polarizability is computed…
Predicting lithium-ion battery lifetime is one of the greatest unsolved problems in battery research right now. Recent years have witnessed a surge in lifetime prediction papers using physics-based, empirical, or data-driven models, most of…
Accurate first-principles calculations for the energies, charge distributions, and spin symmetries of many-electron systems are essential to understand and predict the electronic and structural properties of molecules and materials.…
Cement hydration products were studied as influenced by the hydration conditions (hydration time in liquid phase; relative humidity, RH, in gaseous phase). The formation of calcium hydroxide (portlandite, P) and its transformation to…
The relationship between the shape of a molecule and its chemical reactivity is a central tenet in chemistry. However, the influence of the molecular geometry on reactivity can be subtle and result from several opposing effects. Using a…
By using the direct coexistence method, we have calculated the melting points of ice Ih at normal pressure for three recently proposed water models, namely, TIP3P-FB, TIP4P-FB, and TIP4P-D. We obtained Tm = 216 K for TIP3P-FB, Tm = 242 K…
In this work, an extension of the Madrid-2019 force field is presented. We have added the cations Rb + and Cs + and the anions F$^-$, Br$^-$ and I$^-$. These ions were the remaining alkaline and halogen ions not previously considered in the…
Reverse osmosis and nanofiltration are membrane-based methods that remove solutes from solvent, for instance they remove salts from water (desalination). In these methods, an applied pressure is the driving force for solvent to pass the…
The fully self-consistent $GW$ (sc$GW$) method with the iterative solution of Dyson equation provides a consistent approach for describing the ground and excited states without any dependence on the mean-field reference. In this work, we…
As per the Franck-Condon principle, absorption spectroscopy reveals changes in nuclear geometry in molecules or solids upon electronic excitation. It is often assumed these changes cannot be resolved beyond the ground vibrational…
Salicylidenaniline (SA) is an archetypal system for excited-state intramolecular proton transfer (ESIPT) in non-planar systems. Multiple channels for relaxation involving both the keto and enol forms have been proposed after excitation to…