Developing the MCTDH Quantum Dynamics Code: Accurate Direct Dynamics of Non-Adiabatic Phenomena

开发 MCTDH 量子动力学代码：非绝热现象的精确直接动力学

基本信息

批准号：
EP/K037943/2
负责人：
Graham Worth
金额：
$ 0.43万
依托单位：
University College London
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2016
资助国家：
英国
起止时间：
2016 至无数据
项目状态：
已结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FK037943%2F2
关键词：
Developing MCTDH Quantum Dynamics Code

项目摘要

Understanding the energy flow in molecules after absorbing a photon of light is important to understand their light-activated properties. These are important in a range of technologies, such as harvesting solar energy and data storage, as well as understanding photo-stability and deriving new molecules via photochemical pathways. This energy flow is complex, as a number of different pathways (channels) are available. Of particular importance are what are termed non-adiabatic pathways that allow a molecule to undergo a change of chemical character (electronic state) effectively instantaneously and so dominate the molecular evolution. Unfortunately it is impossible to say a priori which pathways are most important for a particular molecular, and computer simulations have a large role to play in answering this question by modelling the potential energy surfaces and molecular dynamics after excitation.Computer codes for simulating excited-state dynamics are becoming more powerful and useful. However, there is still no code available that can capture all of the quantum mechanical effects required for the often large molecules of interest. The MCTDH package is one of the few codes that is able to treat these problems accurately in a general, user-friendly way. A development part of the code implements a novel method, the DD-vMCG algorithm. This promises to be able to accurately treat the molecules of interest using what is termed direct dynamics, which couples the dynamical simulation of the changes in molecular structure to a separate program that calculates the potential energy surfaces only when required, thus saving much of the work. Initial studies support this.This DD-vMCG code has shown its potential in a number of studies. It now needs to be developed so that it is efficient, easy to use, and can be developed in a sustainable manner. The sustainable development of scientific software is crucial for it to survive and adapt as science progresses. The planned work will ensure that this method will be able to fulfill its potential after many years of development and be used by the scientific community to help understand and engineer how molecules behave and can ultimately be controlled in the presence of light.

了解分子吸收光子后的能量流对于了解其光激活特性非常重要。这些对于一系列技术都很重要，例如收集太阳能和数据存储，以及了解光稳定性和通过光化学途径衍生新分子。这种能量流很复杂，因为有许多不同的路径（通道）可用。特别重要的是所谓的非绝热途径，它允许分子有效地瞬时经历化学特性（电子态）的变化，从而主导分子演化。不幸的是，不可能先验地说哪些途径对于特定分子最重要，并且计算机模拟通过对激发后的势能表面和分子动力学进行建模，在回答这个问题方面发挥着重要作用。用于模拟激发态的计算机代码动态变得更加强大和有用。然而，仍然没有可用的代码可以捕获通常感兴趣的大分子所需的所有量子力学效应。 MCTDH 包是少数能够以通用、用户友好的方式准确处理这些问题的代码之一。代码的开发部分实现了一种新颖的方法，即 DD-vMCG 算法。这有望使用所谓的直接动力学精确处理感兴趣的分子，它将分子结构变化的动态模拟与一个单独的程序结合起来，该程序仅在需要时计算势能表面，从而节省了大量工作。初步研究支持了这一点。该 DD-vMCG 代码已在多项研究中显示出其潜力。现在需要对其进行开发，使其高效、易于使用并且能够以可持续的方式开发。科学软件的可持续发展对于其生存和适应科学进步至关重要。计划的工作将确保这种方法经过多年的发展能够发挥其潜力，并被科学界用来帮助理解和设计分子的行为方式，并最终在光存在下进行控制。