Towards the Development of Reactive Machine-Learned Potentials for Describing Chemistry in Solution

一年级：一般技能培训和实验室轮换2-4年级：MLP是一个令人兴奋的当前研究领域。它们的使用带来的好处(特别是它们摆脱了精度和计算效率之间的根本权衡的能力)使它们成为研究复杂复杂的液相反应的理想工具。现在有机会用“计算显微镜”来研究新的反应现象。这个项目将作为一个概念验证研究，应用反应MLP来描述溶液中的化学。我们将开发一个MLP来精确地模拟水分子体系的静态、动态和反应性质。我们的方法将使用NNPs(具体地说，是一个HD-NNPs委员会)，我们将使用它来提供一个灵活且可扩展的模型，用于模拟不同类型和规模的系统。我们将开发这一NNP，以模拟一系列条件、环境和介质中二氧化碳和水(自然界中的一个基本过程)之间的反应。在进行这项初步研究时，我们希望既获得对我们的研究系统的有价值的见解，同时也改进我们的方法，以扩展到更大和更复杂的反应系统。我们预计，开发这些方法将很快显示出一个新的、通用的框架，用于模拟液体中和界面上的反应，这将在合成化学中被证明是重要的，有助于阐明新的途径、最佳的反应条件，并对控制反应事件的基本原理有新的见解。

Year 1: General skills training and lab rotationsYears 2-4: MLPs are an exciting and current field of research. The benefits afforded by their use (particularly their ability to escape the fundamental trade-off between accuracy and computational efficiency) make them ideal for investigating the complex intricacies of liquid-phase reactions. There is now the opportunity to shine the 'computational microscope' on novel reaction phenomena.This project will functions as a proof-of-concept study for applying reactive MLPs to describing chemistry in solution. We will develop an MLP to accurately model the static, dynamical, and reactive properties of an aqueous system of molecules. Our methodology will employs NNPs (specifically, a committee of HD-NNPs), which we will use to provide a flexible and scalable model for simulating over different system types and sizes. We will develop this NNP towards modelling the reaction between CO2 and H2O (a fundamental process in a nature) across a range of conditions, environments, and media. In conducting this initial research, we hope to both gain valuable insight into our system of study while also improving our methodology for extensions to larger and more complex reactive systems. We anticipate that developing these methods will soon manifest a new, generalised framework for simulating reactions in liquids and at interfaces, which will prove important in synthetic chemistry for elucidating new pathways, optimal reaction conditions, and obtaining new insight into the fundamental principles governing reactive events.