Scalable Quantum Chemistry with Flexible Embedding

我们建议开发和开发一种新的软件，用于复杂体系中的反应性的分子模拟，特别是在水等溶剂存在下的表面化学和多相催化。我们所针对的科学的例子是*在存在或水中工作的金属氧化物催化*污染物物种(重金属或有毒有机物)与环境中的自然矿物的结合，或者特别设计的无机材料，可以潜在地将它们从环境中去除*更复杂的矿物的催化，现有的处理方法不能很好地处理，但具有巨大的工业意义*通过无机表面的有机层设计传感器和光电材料我们将通过结合量子化学(也称为第一原理)技术来实现这一点，该技术可以处理化学反应中心与系统其余部分的经典(或经验)模型(模拟手术的材料平板，以及其上的溶剂层)。我们方法的新奇之处在于，我们在许多重要方面扩展了经典建模环境和量子力学计算之间相互作用的质量。我们正在结合我们自己的一些想法，比如修改现有的模型，以包括自旋极化效应与其他人开发和测试的想法(水分子的冻结电子密度模型)。我们选择开放源代码量子化学程序NWChem作为新功能的基础，因为它是从零开始设计的，用于高性能计算机，并且在设计上是模块化的，将有助于支持我们需要的变化。MM代码(GULP)已经在我们现有的工作中使用，并且在并行机上工作得很好。并行效率是接口代码设计的关键驱动因素，并将指导我们实现新方法的方式。从长远来看，这里开发的代码将基于我们在过去软件项目中获得的经验，形成更广泛系统(包括生物系统)的建模框架的核心。

We propose to develop and a new piece of software for molecular modelling of reactivity in complex systems, in particular, surface chemistry and heterogeneous catalysis in the presence of solvent such as water.Examples of the science we are targetting are * metal oxide catalysis that work in the presence or water * the binding of pollutant species (heavy metals or toxic organics) to natural minerals in the environment, or specially designed inorganic materials that could potentially remove them from the environment * catalysis by more complex minerals, not well treated by existing treatments but of great industrial importance * design of sensors and photoelectric materials by organic layers on inorganic surfacesWe will do this by combining quantum chemistry (also known as first principles) techniques, which can treat the chemically reacting centres with classical (or empirical) models for the rest of the system (the slab of material which is modelling a surgfae, and the solvent layers on top of it.The novelty in our approach is that we are extending the quality of the interaction between the classically modelled environment and the quantum mechanical calculation in a number of significant respects. We are combining some of our own ideas, such as adapting existing models to include spin polarisation effects with ideas (frozen electron density models for water molecules) that have been developed and tested by others.We are choosing an Open Source quantum chemistry program, NWChem as the basis for the new features because it has been designed from scratch for use on high-performance computers, and is modular in design which will help support the changes we need to make. The MM code (GULP) is already used in our existing work, and works well on parallel machines. Parallel efficiency is a key driver for the design of the interfaced code and will inform the way we implement the new methods.In the long run, it is intended the code developed here will form the nucleus of a modelling framework for a wider range of systems (including biological ones) building on experience we have had in past software projects (www.chemshell.org).