相关论文: Ab initio surface chemistry with chemical accuracy
Water interactions with oxygen-deficient cerium dioxide (CeO$_2$) surfaces are central to hydrogen production and catalytic redox reactions, but the atomic-scale details of how defects influence adsorption and reactivity remain elusive.…
We report an investigation of the suitability of quantum embedding for modeling the effects of the environment on the X-ray photoelectron spectra of hydrogen chloride and the chloride ions adsorbed on ice surfaces, as well as of chloride…
Over 90 % of all chemical manufacture uses a solid catalyst. Related work thus responds to major societal demand. This study is of water-gas shift on platinum for hydrogen production. The close-packed Pt(111) surface catalyses this process.…
We present an implementation of equation of motion coupled-cluster singles and doubles (EOM-CCSD) theory using periodic boundary conditions and a plane wave basis set. Our implementation of EOM-CCSD theory is applied to study $F$-centers in…
This study evaluates the precision of widely recognized quantum chemical methodologies, CCSD(T), DLPNO-CCSD(T) and localized ph-AFQMC, for determining the thermochemistry of main group elements. DLPNO-CCSD(T) and localized ph-AFQMC, which…
Clean oxide surfaces are generally hydrophilic. Water molecules anchor at undercoordinated surface metal atoms that act as Lewis-acid sites, and they are stabilized by H bonds to undercoordinated surface oxygens. The large unit cell of…
For a given many-electron molecule, it is possible to define a corresponding one-electron Schr\"odinger equation, using potentials derived from simple atomic densities, whose solution predicts fairly accurate molecular orbitals for single-…
Controlling the water contact angle on a surface is important for regulating its wettability in industrial applications, which involves developing ab initio prediction scheme of accurately predicting the angle. The scheme requires…
We adapt the computational hydrogen electrode approach to explicitly account for photo-generated charges and use it to computationally screen for viable catalyst/co-catalyst combinations for photo-catalytic water splitting. The hole energy…
Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study…
Simulating liquid water to an accuracy that matches its wealth of available experimental data requires both precise electronic structure methods and reliable sampling of nuclear (quantum) motion. This is challenging because applying the…
Understanding molecular adsorption on surfaces underpins many problems in chemistry and materials science. Accurately and efficiently describing the adsorption has been a challenging task for first-principles methods as the process can…
The influences of water molecules surrounding biological molecules during irradiation with heavy particles (atoms,ions) are currently a major subject in radiation science on a molecular level. In order to elucidate the underlying complex…
Every mathematical model describing physical phenomena is an approximation to model reality, hence has its limitations. Depending on characteristic values of the variables in the model, different aspects of the model and, e.g.,…
Simplified, classical models of water are an integral part of atomistic molecular simulations, especially in biology and chemistry where hydration effects are critical. Yet, despite several decades of effort, these models are still far from…
Surface chemistry on interstellar dust grains is recognized as a central component in astrochemical models, representing a plausible formation route for many of the observed complex molecular species. However, key parameters governing…
Difficulties associated with the integration of liquids into a UHV environment make surface-science style studies of mineral dissolution particularly challenging. Recently, we developed a novel experimental setup for the UHV-compatible…
Surface-subsurface flow models for hydrological applications solve a coupled multiphysics problem. This usually consists of some form of the Richards and shallow water equations. A typical setup couples these two nonlinear partial…
An analysis of the values and signs of the activation energies of temperature dependences (TDs) of the self-diffusion coefficient (D) and dynamic viscosity ({\eta}) in the range from 0 {\deg}C to 100 {\deg}C confirmed that the molecular…
Understanding the dehydrogenation of transition metal oxide surfaces under electrochemical potential is critical to the control of important chemical processes such as the oxygen evolution reaction (OER). Using first principles…