标题： 一种用于模拟离子材料表面化学的准确且高效的框架 显示英文标题

标题： An accurate and efficient framework for modelling the surface chemistry of ionic materials

摘要： 量子力学模拟可以提供关于表面化学过程的原子级见解。 这种理解对于合理设计新的固体催化剂以及储存能量和减少温室气体的材料至关重要。 然而，实现可靠预测所需的准确性已被证明具有挑战性。 密度泛函理论（DFT）是常用的量子力学方法，通常会导致不一致的预测，因此需要来自关联波函数理论（cWFT）的准确方法。 然而，与cWFT相关的高计算需求和大量用户干预传统上使其难以用于表面。 在本工作中，我们解决了这一挑战，提出了一种自动化框架，利用多级嵌入方法，将准确的cWFT方法应用于离子材料表面，计算成本接近DFT。 通过这个框架，我们再现了19种不同吸附质-表面系统的实验吸附焓。 此外，我们解决了几个系统吸附构型的争论，同时提供了评估DFT的基准。 该框架是开源的，使得更常规地将cWFT应用于涉及离子材料表面的复杂问题成为可能。 显示英文摘要

摘要： Quantum-mechanical simulations can offer atomic-level insights into chemical processes on surfaces. This understanding is crucial for the rational design of new solid catalysts as well as materials to store energy and mitigate greenhouse gases. However, achieving the accuracy needed for reliable predictions has proven challenging. Density functional theory (DFT), the workhorse quantum-mechanical method, can often lead to inconsistent predictions, necessitating accurate methods from correlated wave-function theory (cWFT). However, the high computational demands and significant user intervention associated with cWFT have traditionally made it impractical to carry out for surfaces. In this work, we address this challenge, presenting an automated framework which leverages multilevel embedding approaches, to apply accurate cWFT methods to the surfaces of ionic materials with computational costs approaching DFT. With this framework, we have reproduced experimental adsorption enthalpies for a diverse set of 19 adsorbate-surface systems. Moreover, we resolve debates on the adsorption configuration of several systems, while offering benchmarks to assess DFT. This framework is open-source, making it possible to more routinely apply cWFT to complex problems involving the surfaces of ionic materials.