相关论文: Quantum Delocalization Enables Water Dissociation …
We have employed the highly accurate complex absorbing potential based ionization potential equation-of-motion coupled cluster singles and doubles (CAP-IP-EOM-CCSD) method to study the various intermolecular decay processes in ionized…
Second-Harmonic Scatteringh (SHS) experiments provide a unique approach to probe non-centrosymmetric environments in aqueous media, from bulk solutions to interfaces, living cells and tissue. A central assumption made in analyzing SHS…
We introduce machine learning models of quantum mechanical observables of atoms in molecules. Instant out-of-sample predictions for proton and carbon nuclear chemical shifts, atomic core level excitations, and forces on atoms reach…
Quantum computing leverages the quantum resources of superposition and entanglement to efficiently solve computational problems considered intractable for classical computers. Examples include calculating molecular and nuclear structure,…
Nuclear quantum effects (NQEs) on the structures and transport properties of dense liquid hydrogen at densities of 10-100 g/cm3 and temperatures of 0.1-1 eV are fully assessed using \textit{ab initio} path-integral molecular dynamics…
Water is often viewed as a collection of monomers interacting electrostatically with each other. We compare the water proton momentum distributions from recent neutron scattering data with those calculated from two electronic structure…
An inhomogeneous electric field is used to study the deflection of a supersonic beam of water molecules. The deflection profiles show strong broadening accompanied by a small net displacement towards higher electric fields. The profiles are…
We discuss the role of water bridging the DNA-enzyme interaction by resorting to recent results showing that London dispersion forces between delocalized electrons of base pairs of DNA are responsible for the formation of dipole modes that…
We propose a strategy for enabling photodissociation of a normally photostable molecule through coupling to a nanoparticle plasmon. The large possible coupling on the single-molecule level combined with the highly lossy nature of plasmonic…
We study alchemical atomic energy partitioning as a method to estimate atomisation energies from atomic contributions which are defined in physically rigorous and general ways through use of the uniform electron gas as a joint reference. We…
Equilibration dynamics of hot oxygen atoms following O2 dissociation on Pd(100) and Pd(111) surfaces are investigated by molecular dynamics simulations based on a scalable neural network potential enabling first-principles description of O2…
A ubiquitous approach to obtain transferable machine learning-based models of potential energy surfaces for atomistic systems is to decompose the total energy into a sum of local atom-centred contributions. However, in many systems…
Water-metal interfaces are ubiquitous and play a key role in many chemical processes, from catalysis to corrosion. Whereas water adlayers on atomically flat transition metal surfaces have been investigated in depth, little is known about…
Despite the simplicity of its molecular unit, water is a challenging system because of its uniquely rich polymorphism and predicted but yet unconfirmed features. Introducing a novel space of generalized coordinates that capture changes in…
Crystal nucleation is relevant across the domains of fundamental and applied sciences. However, in many cases its mechanism remains unclear due to a lack of temporal or spatial resolution. To gain insights to the molecular details of…
The interaction of water with Fe$_3$O$_4$(001) is studied by density functional theory (DFT) calculations including an on-site Coulomb term. For isolated molecules dissociative adsorption is strongly promoted at surface defect sites, while…
We show how machine learning techniques based on Bayesian inference can be used to reach new levels of realism in the computer simulation of molecular materials, focusing here on water. We train our machine-learning algorithm using…
Water freezing is ubiquitous on Earth, affecting many areas from biology to climate science and aviation technology. Probing the atomic structure in the homogeneous ice nucleation process from scratch is of great value but still…
The results of studies on the properties of ordinary and heavy water subjected to sharp mechanical impacts at acoustic repetition frequency are presented. Experimental evidence for the phenomenon of acoustically induced nuclear processes in…
Oxide-water interfaces govern a wide range of physical and chemical processes fundamental to many fields like catalysis, geochemistry, corrosion, electrochemistry, and sensor technology. Near solid oxide surfaces, water behaves differently…