A Joined-up Approach for New Molecular Simulation Technologies To Harness Ultrafast Photochemistry

光引发许多重要的化学反应。这些包括光合作用，它将阳光转化为化学能并为地球上大多数生命提供动力，人类视觉，其中使用我们视网膜中分子的光诱导异构化来检测光，以及新技术，如癌症的光动力疗法，分子光子学，光子学和有机发光二极管显示器。研究这类过程的超快成像实验依赖于计算建模来解释和分析数据，并从观察中提取化学和物理见解。然而，计算建模仍然非常具有挑战性，本质上是因为在光化学过程中被分子吸收的光子（“光粒子”）携带大量能量，这迫使电子和原子核进入量子力学描述的复杂耦合运动，使得计算比经典力学描述的相应系统更困难。必要的计算由两种不同类型的计算组成，这两种计算都需要大量的技术专长：电子结构计算和量子动力学。我们将联合收割机结合我们在电子结构计算和量子动力学方面的专业知识，创造强大的新模拟方法。该团队包括两名世界领先的实验学家，他们都是互补超快成像技术的专家。作为一个团队，我们将推动实验和理论，以实现更深入地了解分子中复杂的光激活动力学。该项目将为解释多个互补的最先进的实验提供一个框架。长期目标是实现足够强大的模拟，以便我们可以使用计算机为新的光驱动技术设计新的光敏分子。在该项目的后期阶段，我们将处理远远超出当前模拟前沿的复杂分子系统，其中将包括令人兴奋的应用，如光敏剂，光稳定剂，光敏前药，光敏剂，光催化剂和发光二极管。

Light triggers many important chemical reactions. These include photosynthesis, which converts sunlight to chemical energy and powers most life on earth, human vision, where light is detected using the light-induced isomerisation of a molecule in our retinas, and new technologies such as photodynamic therapies for cancer, photocatalysis, molecular photonics, photovoltaics, and organic light-emitting diodes in displays. Ultrafast imaging experiments that study these types of processes rely on computational modelling to interpret and analyse data and extract chemical and physical insight from the observations. Yet, the computational modelling remains very challenging, in essence because the photon ('light-particle') absorbed by a molecule in a photochemical process carries a large amount of energy, which forces the electrons and nuclei into complex coupled motion described by quantum mechanics, making computations exponentially more difficult than the corresponding system described by classical mechanics. The necessary calculations are composed of two different types of computations, which both require great technical expertise: electronic structure calculations and quantum dynamics. We will combine our expertise in electronic structure calculations and quantum dynamics, to create powerful new simulation methods. The team includes two world-leading experimentalists who are each expert in a complementary ultrafast imaging technique. As a team, we will push experiments and theory to achieve greater insight into complex light-activated dynamics in molecules. The project will provide a framework for interpreting multiple complementary state-of-the-art experiments. The long-term goal is to achieve simulations that are sufficiently powerful that we can use computers to design new photoactive molecules for new light-driven technologies. In the later stages of the project, we will tackle complex molecular systems well beyond the current cutting-edge of simulations, which will include exciting applications such as photosensitizers, photostabilizers, photoactive pro-drugs, photovoltaics, photocatalysts, and light-emitting diodes.