Ultra-fast interfacial charge transfer probed using a core-hole clock implementation of resonant inelastic x-ray scattering (RIXS)

使用共振非弹性 X 射线散射 (RIXS) 的芯孔时钟实现探测超快界面电荷转移

• 批准号: EP/T004355/1
• 负责人: James O'Shea
• 金额: $ 2.67万
• 依托单位: University of Nottingham
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2019
• 资助国家: 英国
• 起止时间: 2019 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FT004355%2F1
• 关键词: Ultra; fast; interfacial; charge; transfer

Ultra-fast electron transfer between a molecule and a surface to which it is coupled plays a key role in light-harvesting devices such as dye-sensitised solar cells and water-splitting photoelectrochemical cells (the model water splitting photoanode shown in figure 1 being a prime example). An elegant way to probe these charge transfer processes, which typically happen on the low femtosecond timescale is the use of resonant core-level spectroscopy in the form of resonant photoemission (RPES). This non-radiative core-hole decay technique relies on monitoring the photoelectrons emitted when a resonantly excited electron participates in the core-hole decay. But these have a very limited escape depth so the technique can only be applied to systems where the charge transfer interface is the surface. In principle, the photons emitted during core-hole decay carry the same information. The corresponding radiative technique is known as resonant inelastic x-ray scattering (RIXS).The aim of this proposal is to realise a novel core-hole clock implementation of resonant inelastic x-ray scattering (RIXS) to probe the electron transfer from specific unoccupied molecular orbitals of a dye molecule into the conduction band of a surface to which it is adsorbed. Using this method we should be able to probe charge transfer dynamics on the timescale of the core-hole lifetime (a few femtoseconds) in the same way as resonant photoemission (RPES), only here we are using a photons-in, photons-out technique. This approach is a very promising route to probing ultra-fast charge transfer in realistic systems where the charge transfer interface of molecular devices such as solar cells are typically buried by a transport layer or electrolyte. The series of synchrotron experiments described in this overseas travel grant proposal aim to obtain the data for a definitive reconciliation of the core-hole clock implementations of both RPES and RIXS, and the application of the latter to a buried charge transfer interface.

分子与其耦合的表面之间的超快速电子转移在光捕获设备中起着关键作用，例如染料敏化太阳能电池和水裂解光电化学电池（图1所示的模型水裂解光电阳极是一个主要例子）。探测这些通常发生在低飞秒时间尺度上的电荷转移过程的一种优雅的方法是使用共振光电发射（RPES）形式的共振芯能级光谱。这种非辐射芯-空穴衰减技术依赖于监测当共振激发的电子参与芯-空穴衰减时发射的光电子。但是这些具有非常有限的逃逸深度，因此该技术只能应用于电荷转移界面是表面的系统。原则上，在核心-空穴衰变期间发射的光子携带相同的信息。相应的辐射技术被称为共振非弹性X射线散射（RIXS）。该建议的目的是实现一种新的核孔时钟实现共振非弹性X射线散射（RIXS）探测电子转移从特定的未占分子轨道的染料分子到其吸附表面的导带。使用这种方法，我们应该能够以与共振光电发射（RPES）相同的方式探测芯孔寿命（几飞秒）时间尺度上的电荷转移动力学，只是在这里我们使用光子输入，光子输出技术。这种方法是一个非常有前途的路线，探测超快的电荷转移在现实系统中的电荷转移界面的分子器件，如太阳能电池通常被掩埋的传输层或电解质。在这个海外旅行补助金提案中描述的一系列同步加速器实验的目的是获得数据，以确定RPES和RIXS的核孔时钟实现的和解，以及后者在掩埋电荷转移界面的应用。

项目成果

The adsorption and XPS of triphenylamine-based organic dye molecules on rutile TiO2(110) prepared by UHV-compatible electrospray deposition

• DOI: 10.1016/j.susc.2023.122323
• 发表时间: 2023-05
• 期刊: Surface Science
• 影响因子: 1.9
• 作者: Nouf Alharbi;Jack Hart;James N. O'Shea

A soft x-ray probe of a titania photoelectrode sensitized with a triphenylamine dye.

用三苯胺染料敏化的二氧化钛光电极的软 X 射线探针。

• DOI: 10.1063/5.0050531
• 发表时间: 2021
• 期刊: The Journal of chemical physics
• 作者: Temperton RH

Ultra-fast charge transfer between fullerenes and a gold surface, as prepared by electrospray deposition

通过电喷雾沉积制备的富勒烯和金表面之间的超快电荷转移

• DOI: 10.1016/j.cplett.2020.137309
• 发表时间: 2020
• 期刊: Chemical Physics Letters
• 影响因子: 2.8
• 作者: Temperton R

Resonant inelastic X-ray scattering of a Ru photosensitizer: Insights from individual ligands to the electronic structure of the complete molecule.

Ru 光敏剂的共振非弹性 X 射线散射：从单个配体到整个分子的电子结构的见解。

• DOI: 10.1063/1.5114692
• 发表时间: 2019
• 期刊: The Journal of chemical physics
• 作者: Temperton RH