Harnessing vibration-induced enhancement of transport in functional materials with soft structural dynamics

利用振动引起的软结构动力学功能材料的输运增强

• 批准号: EP/W017091/1
• 负责人: Henning Sirringhaus
• 金额: $ 872.38万
• 依托单位: University of Cambridge
• 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%2FW017091%2F1
• 关键词: Harnessing; vibration; induced; enhancement; transport

In inorganic semiconductors, such as silicon, the interaction of electronic excitations with lattice vibrations is an undesirable perturbation; it limits charge carrier mobilities and mediates non-radiative recombination. In low-dimensional functional materials with non-covalent bonding the structural dynamics is not a mere perturbation, it moves centre-stage: Some vibrational modes are very soft and strongly anharmonic so that electronic processes occur in a strongly fluctuating structural landscape. The traditional view is that the resulting strong electron-vibrational coupling is also detrimental: In organic semiconductors (OSCs), for example, electronic charges and neutral electron-hole pairs (excitons) are localized by a 'cloud' of lattice deformations, which causes charge mobilities and exciton diffusion lengths to be undesirably small, thus limiting performance of optoelectronic devices. We have recently discovered systems in which this traditional paradigm does not hold, but in which the structural dynamics is highly beneficial and mediates surprisingly fast, long-range excitation transport. This runs completely against models developed for traditional semiconductors such as silicon, for which phonons limit electronic transport. The mechanism involves vibrational modes coupling localized states near the band edges to highly delocalised states within the bands that can then transport charges and energy over unprecedentedly long length scales. This unique transient delocalization regime, in which excitations are effectively able to "surf on the waves" of structural lattice distortions, is not found in silicon and was first discovered in OSCs. Our goal is to explore similar physics in other functional materials with soft structural dynamics, such as hybrid organic-inorganic perovskite (HOIP) semiconductors, 2D conjugated covalent/metal organic frameworks (COFs/MOFs) and inorganic ceramics and ion conductors.VISION AND AMBITION: In the proposed programme we aim to pursue this vibration-enhanced transport (VET) regime as a general paradigm for achieving fast and long-range electronic charge, ion and energy transport in a broad class of organic and inorganic, functional materials with soft structural dynamics. We will (i) develop new experimental/theoretical methodologies to achieve a deep fundamental understanding of the underpinning mechanisms for the vibration-enhanced transport, including identification and molecular engineering of the most effective vibrational modes mediating it, (ii) design new self-assembled functional materials in which transport length scales exceeding micrometers are achievable and (iii) exploit such long length scales to enable new device architectures and transformational device performance improvements in a broad range of (bio)electronic, optoelectronic, energy storage and photocatalytic applications.

在无机半导体（例如硅）中，电子激发与晶格振动的相互作用是一种不良的扰动。它限制了电荷载体的迁移率并介导非辐射重组。在具有非共价键合的低维功能材料中，结构动力学不仅仅是扰动，它可以移动中心阶段：某些振动模式非常柔软且强烈地静脉，因此电子过程在强烈波动的结构景观中发生。传统观点是，产生的强电子振动耦合也有害：例如，在有机半导体（OSC）中，电子电荷和中性电子孔对（激子）被定位为lattice变形的“云”，从而导致电荷动力和激动体的差异长度，从而使得iNDO较小，从而占据了限制。我们最近发现了这种传统范式不存在的系统，但是结构动力学是非常有益的，并介导了令人惊讶的快速，远程激发传输。这完全与针对传统半导体（例如硅）开发的模型，该模型限制了电子传输。该机制涉及振动模式，将带边缘附近的局部状态耦合到频段内的高度离驱域状态，然后可以在前所未有的长度尺度上传输电荷和能量。这种独特的瞬时离域机制在硅中没有发现激发有效地“在结构晶格扭曲的波浪上”的“冲浪”，并且在OSC中最初是在OSC中发现的。我们的目标是探索具有软结构动力学的其他功能材料中的类似物理学，例如混合有机无机钙钛矿（HOHIP）半导体，2D共轭共价/金属有机框架（COFS/MOFS）（COFS/MOFS）和无机陶瓷和INION CONTRAGION。作为在具有软结构动力学的大量有机和无机的功能材料中，作为实现快速和远程电子电荷的一般范式，离子和能量传输。我们将（i）开发新的实验/理论方法，以深入了解振动增强运输的基础机制，包括介导IT的最有效振动模式的识别和分子工程，（ii）设计新的自动组合功能，以超过型号的范围延伸量尺度，以实现的范围超过实现Microter and face-III和III II II II III和（III II II II II II II III），并转换设备的性能改进（BIO）电子，光电，能源存储和光催化应用。

项目成果

Pulsed transistor operation enables miniaturization of electrochemical aptamer-based sensors.

• DOI: 10.1126/sciadv.add4111
• 发表时间: 2022-11-18
• 期刊: Science advances
• 影响因子: 13.6

Pulsed transistor operation enables miniaturization of electrochemical aptamer-based sensors

脉冲晶体管操作使基于电化学适体的传感器小型化

• DOI: 10.17863/cam.91888
• 发表时间: 2022
• 作者: Bidinger S

Direct observation of ultrafast singlet exciton fission in three dimensions.

• DOI: 10.1038/s41467-022-33647-5
• 发表时间: 2022-10-10
• 期刊: Nature communications
• 影响因子: 16.6

Organic Photovoltaic Materials for Solar Fuel Applications: A Perfect Match?

• DOI: 10.1021/acs.chemmater.3c02286
• 发表时间: 2024-02
• 期刊: Chemistry of Materials
• 影响因子: 8.6
• 作者: Catherine M. Aitchison;Iain McCulloch

A 19% efficient and stable organic photovoltaic device enabled by a guest nonfullerene acceptor with fibril-like morphology

• DOI: 10.1039/d2ee03483b
• 发表时间: 2023-01-06
• 期刊: ENERGY & ENVIRONMENTAL SCIENCE
• 影响因子: 32.5
• 作者: Chen, Hu;Jeong, Sang Young;Lin, Yuanbao
• 通讯作者: Lin, Yuanbao