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

利用新分子模拟技术的联合方法来利用超快光化学

• 批准号: EP/V006746/1
• 负责人: Martin Paterson
• 金额: $ 66.82万
• 依托单位: Heriot-Watt University
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2021
• 资助国家: 英国
• 起止时间: 2021 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FV006746%2F1
• 关键词: Joined; up; Approach; New; Molecular

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.

光会引发许多重要的化学反应。这些技术包括光合作用，它将阳光转化为化学能，并为地球上的大多数生命提供动力；人类视觉，通过光诱导视网膜中的分子异构化来检测光；以及新技术，如癌症的光动力学疗法、光催化、分子光子学、光伏技术和显示器中的有机发光二极管。研究这类过程的超快成像实验依赖于计算模型来解释和分析数据，并从观测中提取化学和物理见解。然而，计算模型仍然非常具有挑战性，本质上是因为分子在光化学过程中吸收的光子(光粒子)携带大量能量，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要困难得多。必要的计算由两种不同类型的计算组成，这两种计算都需要很高的技术专长：电子结构计算和量子动力学。我们将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者，他们各自都是互补的超快成像技术方面的专家。作为一个团队，我们将推动实验和理论，以实现对分子中复杂的光激活动力学的更深入的了解。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活性分子。在项目的后期阶段，我们将处理复杂的分子系统，远远超出目前模拟的前沿，其中将包括令人兴奋的应用，如光敏剂、光稳定剂、光活性前体药物、光伏、光催化剂和发光二极管。

项目成果

Protocols for Understanding the Redox Behavior of Copper-Containing Systems.

• DOI: 10.1021/acsomega.2c05484
• 发表时间: 2022-12-13
• 期刊: ACS OMEGA
• 影响因子: 4.1
• 作者: Malcomson, Thomas;Repiscak, Peter;Erhardt, Stefan;Paterson, Martin J.
• 通讯作者: Paterson, Martin J.

The Value of Different Experimental Observables: A Transient Absorption Study of the Ultraviolet Excitation Dynamics Operating in Nitrobenzene.

• DOI: 10.1021/acs.jpca.3c02654
• 发表时间: 2023-08-10
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY A
• 影响因子: 2.9
• 作者: Crane, Stuart W.;Garrow, Malcolm;Lane, Paul D.;Robertson, Kate;Waugh, Alex;Woolley, Jack M.;Stavros, Vasilios G.;Paterson, Martin J.;Greaves, Stuart J.;Townsend, Dave
• 通讯作者: Townsend, Dave

The Photochemical Mediated Ring Contraction of 4H-1,2,6-Thiadiazines To Afford 1,2,5-Thiadiazol-3(2H)-one 1-Oxides.

• DOI: 10.1021/acs.orglett.3c02673
• 发表时间: 2023-09-22
• 期刊: ORGANIC LETTERS
• 影响因子: 5.2
• 作者: Broumidis, Emmanouil;Thomson, Christopher G.;Gallagher, Brendan;Sotorrios, Lia;Mckendrick, Kenneth G.;Macgregor, Stuart A.;Paterson, Martin J.;Lovett, Janet E.;Lloyd, Gareth O.;Rosair, Georgina M.;Kalogirou, Andreas S.;Koutentis, Panayiotis A.;Vilela, Filipe
• 通讯作者: Vilela, Filipe

Efficient Computation of Two-Electron Reduced Density Matrices via Selected Configuration Interaction.

通过选定的配置相互作用有效计算二电子约简密度矩阵。

• DOI: 10.1021/acs.jctc.2c00738
• 发表时间: 2022-11-08
• 期刊: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
• 影响因子: 5.5
• 作者: Coe, Jeremy P.;Carrascosa, Andres Moreno;Simmermacher, Mats;Kirrander, Adam;Paterson, Martin J.
• 通讯作者: Paterson, Martin J.

A Concerted Redox- and Light-Activated Agent for Controlled Multimodal Therapy against Hypoxic Cancer Cells.

用于针对缺氧癌细胞的受控多模式治疗的协同氧化还原和光激活剂。

• DOI: 10.1002/adma.202210363
• 发表时间: 2023
• 期刊: Advanced materials (Deerfield Beach, Fla.)
• 作者: Liu J