Excited state dynamics of shape-shifting molecules

变形分子的激发态动力学

基本信息

批准号：
EP/W018691/1
负责人：
James Bull
金额：
$ 59.49万
依托单位：
University of East Anglia
依托单位国家：
英国
项目类别：
Research Grant
财政年份：
2022
资助国家：
英国
起止时间：
2022 至无数据
项目状态：
未结题

来源：
https://gtr.ukri.org/projects?ref=EP%2FW018691%2F1
关键词：
Excited state dynamics shape shifting

项目摘要

Molecules that change shape (isomerise) in response to light are essential in numerous light-controlled technological applications including optical memory registers, advanced materials and nanotechnological molecular machines capable of performing specific tasks at the microscopic level. In addition to their technological applications, shape-changing 'photoswitch' molecules have widespread biological importance, including roles in vision, phototropism and photosynthesis in bacteria, and ion channel switches. The shape-shifting properties of these photoswitch molecules stems from the existence of two or more distinct isomers that can be toggled following exposure to different colours of light. Each isomer may have unique properties, including molecular volume, colour, solubility, and conductivity.Improving our molecular-level understanding of the actinic mechanistic details of photoswitching - the so-called excited state dynamics - is critical for the rational design of improved derivatives. Harnessing this knowledge is becoming increasingly important due to the widespread adoption of photoswitches into everyday life, requiring new spectroscopic methodologies that offer increased selectivity and information content. In particular, the spectroscopic toolkit must have the capacity to independently probe the excited state dynamics associated with each isomer, which invariably occurs over the ultrafast femtosecond (0.000000000000001 second) timescale, and also the capacity to characterise branching to multiple photoswitch forms or degradation pathways. It is often difficult or impossible to characterise the inherent photoswitching properties of each isomer using conventional analytical or physical chemistry techniques, particularly when there are several isomers, rapid interconversion and strong environmental influences. This research program will develop new vacuum-based instrumentation and methodology to help address these deficiencies and will focus on applying the toolkit to characterising two classes of molecular photoswitches important in optoelectronics and optical control of biotechnological molecules.Building on our unique expertise gained from multiple world-leading laboratories, this research program will establish long-term research infrastructure in the UK, permitting study of shape-selected molecules and their ultrafast shape-shifting dynamics. The instrumentation and methodology will provide a distinctive new approach and offer end capabilities that are not possible by any other single research group.

在众多光照控制的技术应用中，必须改变形状的分子（异构体）是必不可少的，包括光学记忆寄存器，高级材料和能够在微观级别执行特定任务的纳米技术分子机器。除了其技术应用外，变化形状的“ Photoswitch”分子具有广泛的生物学重要性，包括在视觉，细菌中的光质主义和光合作用中的作用，以及离子通道开关。这些Photoswitch分子的形状转移特性源于存在两个或更多不同的异构体，这些异构体可以在暴露于不同颜色的光线后切换。每个异构体可能具有独特的特性，包括分子体积，颜色，溶解度和电导率。对分子级别的理解进行了对照片处理的光化机械细节的理解 - 所谓的激发态动力学 - 对于改善衍生物的合理设计至关重要。由于广泛采用照片开关融入日常生活中，因此利用这些知识变得越来越重要，需要新的光谱方法，这些方法论可以提高选择性和信息内容。特别是，光谱工具包必须具有独立探测与每个异构体相关的激发状态动力学的能力，而这些动力学与每个异构体相关的激发状态动力学总是发生在超快的飞秒（0.000000000000001秒）上的时间表，并且还具有将分支到多个Photoswitch形式或降级途径的分支的能力。使用常规的分析或物理化学技术来表征每个异构体的固有照片处理特性通常很难或不可能，尤其是在存在几种异构体，快速互转换和强烈的环境影响时。该研究计划将开发新的基于真空的仪器和方法，以帮助解决这些缺陷，并将专注于应用工具包来表征两类在光电学中重要的分子照片开关以及对生物技术分子的光学控制。建立我们在多个世界领域的研究方面的独特专业知识，将在多个世界领导的实验室中获得允许，以建立多个世界实施的实施范围，从而建立成型的实施范围。分子及其超快形状转移动力学。仪器和方法论将提供一种独特的新方法，并提供任何其他单一研究小组无法实现的最终功能。

项目成果

期刊论文数量（10）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Cooling dynamics of energized naphthalene and azulene radical cations

DOI：
10.1063/5.0147456
发表时间：
2023-05-07
期刊：
JOURNAL OF CHEMICAL PHYSICS
影响因子：
4.4
作者：
Lee, Jason W. L.;Stockett, Mark H. H.;Bull, James N. N.
通讯作者：
Bull, James N. N.

Cryogenic Fluorescence Spectroscopy of Ionic Fluorones in Gaseous and Condensed Phases: New Light on Their Intrinsic Photophysics.

DOI：
10.1021/acs.jpca.2c07231
发表时间：
2022-12
期刊：
The journal of physical chemistry. A
影响因子：
0
作者：
Eleanor K Ashworth;J. Langeland;M. Stockett;T. T. Lindkvist-T.;Christina Kjær;J. Bull;S. Nielsen
通讯作者：
Eleanor K Ashworth;J. Langeland;M. Stockett;T. T. Lindkvist-T.;Christina Kjær;J. Bull;S. Nielsen

Statistical vibrational autodetachment and radiative cooling rates of para-benzoquinone.

对苯醌的统计振动自脱离和辐射冷却速率。