相关论文: Ab initio surface chemistry with chemical accuracy
Quantitative prediction of thermodynamic properties in solution is essential for translating atomistic simulations into reliable chemical insight. As an exemplar system, the behaviour of CaCO$_3$ in water has been widely studied to…
Modern electronic structure theories can predict and simulate a wealth of phenomena in surface science and solid-state physics. In order to allow for a direct comparison with experiment, such ab initio predictions have to be made in the…
Predictive simulation of surface chemistry is of paramount importance for progress in fields from catalysis to electrochemistry and clean energy generation. Ab-initio quantum many-body methods should be offering deep insights into these…
First-principles density-functional theory and supercell models are employed to calculate the adsorption of water molecules on the Cu(100) surface. In agreement with the experimental observations, the calculations show that a H2O molecule…
The adsorption of CO on the surface of MgO has long been a model problem in surface chemistry. Here, we report periodic Gaussian-based calculations for this problem using second-order perturbation theory (MP2) and coupled-cluster theory…
In order to rigorously evaluate the energy and dipole moment of a certain configuration of molecules one needs to solve the Schr\"odinger equation. Repeating this for many different configurations allows one to determine the potential…
Using a new form of density functional theory for the {\em ab initio} description of electronic systems in contact with a dielectric environment, we present the first detailed study of the impact of a solvent on the surface chemistry of…
A first-principles study of the adsorption of a single water molecule on a layer of graphitic carbon nitride employing an embedding approach is presented. The embedding approach involves an algorithm to obtain localized Wannier orbitals of…
The interaction of water with $\alpha$-alumina (i.e. $\alpha$-Al$_{2}$O$_{3}$ surfaces is important in a variety of applications and a useful model for the interaction of water with environmentally abundant aluminosilicate phases. Despite…
We present a general theory to treat periodic solids with quantum-chemistry methods. It relies on two main developments: 1) the modeling of a solid as a Clifford torus which is a torus that is both periodic and flat and 2) the introduction…
We present quantum dynamical calculations that describe the rotational excitation of H$_2$O due to collisions with H atoms. We used a recent, high accuracy potential energy surface, and solved the collisional dynamics with the…
By judicious use of extrapolations to the 1-particle basis set limit and $n$-particle calibration techniques, total atomization energies of molecules with up to four heavy atoms can be obtained with calibration accuracy (1 kJ/mol or better,…
We present a comprehensive benchmark study of the adsorption energy of a single water molecule on the (001) LiH surface using periodic coupled cluster and quantum Monte Carlo theories. We benchmark and compare different implementations of…
We report an ab initio evaluation of the surface energy of a simple metal, performed via a coupling-constant integration over the dynamical density-response function. The rapid rate of change of the electron density at the surface is…
We present a general computational scheme based on molecular dynamics (m.d.) simulation for calculating the chemical potential of adsorbed molecules in thermal equilibrium on the surface of a material. The scheme is based on the calculation…
Coupled-cluster theory with single, double, and perturbative triple excitations (CCSD(T)) -- often considered the "gold standard" of main-group quantum chemistry -- is inapplicable to three-dimensional metals due to an infrared divergence,…
Ab initio modeling of electrochemical systems is becoming a key tool for understanding and predicting electrochemical behavior. Development and careful benchmarking of computational electrochemical methods are essential to ensure their…
Bimetallic alloys have drawn extensive attentions in materials science due to their widespread applications in electronics, engineering and catalysis. A very fundamental question of alloy is its surface segregation phenomenon. Many recent…
Although liquid water is ubiquitous in chemical reactions at roots of life and climate on the earth, the prediction of its properties by high-level ab initio molecular dynamics simulations still represents a formidable task for quantum…
Finding accurate solutions to the Schr\"odinger equation is the key unsolved challenge of computational chemistry. Given its importance for the development of new chemical compounds, decades of research have been dedicated to this problem,…