相关论文: Quantum Monte Carlo method for metal catalysis: ca…
Hydrogen production as a clean, sustainable replacement for fossil fuels is gathering pace. Doubling the capacity of Paris-CDG airport has been halted, even with the upcoming Olympic Games, until hydrogen powered planes can be used. It is…
Hydrogen synthesis is a clean, sustainable alternative to fossil fuel \cite{gals}. It has come of age: prototyping various aspects of hydrogen power are hot topics. In 9 out of 10 reactions, a solid catalyst is used. Here hydrogen…
The yardstick of new first-principles approaches to key points on reaction paths at metal surfaces is chemical accuracy compared to reliable experiment. By this we mean that such values as the activation barrier are required to within 1…
The present letter describes an atomic scale investigation of a chemical reaction for selective hydrogen production. This clean fuel is a sustainable energy source. Because electron transfer is the key to such reactions, accurate methods…
Many chemical reactions involve bond-dissociation. This is also true for reactions at solid surfaces, in which the dissociation step is often limiting but facilitated in comparison to gas phase reaction channels. This work considers…
Hydrogen production as a clean, sustainable replacement for fossil fuels is gathering pace. Doubling the capacity of Paris-CDG airport has been halted, even with the upcoming Olympic Games, until hydrogen-powered planes can be used. It is…
The yardstick of new first-principles approaches to key points on reaction paths at metal surfaces is chemical accuracy compared to reliable experiment. By this we mean that such values as the activation barrier are required to within 1…
Nowadays, there is pressing demand for sustainable energy sources, or clean and 'green' fuel and hydrogen is a perfect candidate. It can be made by dissociating methane with the energy input compensated by metal-hydrogen bond formation.…
We present a multi-lattice kinetic Monte Carlo (kMC) approach that efficiently describes the atomistic dynamics of morphological transitions between commensurate structures at crystal surfaces. As an example we study the reduction of a…
We use the diffusion quantum Monte Carlo (DMC) method to calculate the ground state phase diagram of solid molecular hydrogen and examine the stability of the most important insulating phases relative to metallic crystalline molecular…
The precise understanding of adsorption energetics and molecular geometry at catalytic sites is fundamental for advancing catalysis, particularly under the constraints of resource efficiency and environmental sustainability. This study…
Electronic structure of the manganese oxide solid is studied by the quantum Monte Carlo (QMC) methods. The trial wavefunctions are built using orbitals from unrestricted Hartree-Fock and Density Functional Theory, and the electron-electron…
We describe a first-principles statistical mechanics approach enabling us to simulate the steady-state situation of heterogeneous catalysis. In a first step density-functional theory together with transition-state theory is employed to…
Silica is an abundant component of the Earth whose crystalline polymorphs play key roles in its structure and dynamics. As the simplest silicates, understanding pure silica is a prerequisite to understanding the rocky part of the Earth, its…
We perform quantum Monte Carlo (QMC) calculations to determine minimum energy pathways of simple chemical reactions, and compare the computed geometries and reaction barriers with those obtained with density functional theory (DFT) and…
We apply diffusion quantum Monte Carlo (DMC) to a broad set of solids, benchmarking the method by comparing bulk structural properties (equilibrium volume and bulk modulus) to experiment and DFT based theories. The test set includes…
We investigate the binding of single and quadruple hydrogen molecules on a positively charged Ca ion. By comparing with benchmark quantum Monte Carlo (QMC) calculations we demonstrate wide variability in other more approximate electronic…
Quantum Monte Carlo (QMC) methods represent a powerful family of computational techniques for tackling complex quantum many-body problems and performing calculations of stationary state properties. QMC is among the most accurate and…
Density functional theory (DFT) is widely used in surface science, but gives poor accuracy for oxide surface processes, while high-level quantum chemistry methods are hard to apply without losing basis-set quality. We argue that quantum…
Describing correlated electron systems near phase transitions has been a major challenge in computational condensed-matter physics. In this paper, we apply highly accurate fixed node quantum Monte Carlo techniques, which directly work with…