Cassabaum Alyssa A, Bera Kajari, Rich Christopher C, Nebgen Bailey R, Kwang Siu Yi, Clapham Margaret L, Frontiera Renee R
Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, USA.
J Chem Phys. 2020 Jul 21;153(3):030901. doi: 10.1063/5.0009976.
Femtosecond stimulated Raman spectroscopy (FSRS) is a chemically specific vibrational technique that has the ability to follow structural dynamics during photoinduced processes such as charge transfer on the ultrafast timescale. FSRS has a strong background in following structural dynamics and elucidating chemical mechanisms; however, its use with solid-state materials has been limited. As photovoltaic and electronic devices rely on solid-state materials, having the ability to track the evolving dynamics during their charge transfer and transport processes is crucial. Following the structural dynamics in these solid-state materials will lead to the identification of specific chemical structures responsible for various photoinduced charge transfer reactions, leading to a greater understanding of the structure-function relationships needed to improve upon current technologies. Isolating the specific nuclear motions and molecular structures that drive a desired physical process will provide a chemical blueprint, leading to the rational design and fabrication of efficient electronic and photovoltaic devices. In this perspective, we discuss technical challenges and experimental developments that have facilitated the use of FSRS with solid-state samples, explore previous studies that have identified structure-function relationships in charge transfer reactions, and analyze the future developments that will broaden and advance the field.
飞秒受激拉曼光谱（FSRS）是一种具有化学特异性的振动技术，能够在超快时间尺度上追踪光诱导过程（如电荷转移）中的结构动力学。FSRS在追踪结构动力学和阐明化学机制方面有很强的背景；然而，它在固态材料中的应用一直有限。由于光伏和电子器件依赖于固态材料，能够在其电荷转移和传输过程中追踪不断演变的动力学至关重要。追踪这些固态材料中的结构动力学将有助于识别导致各种光诱导电荷转移反应的特定化学结构，从而更深入地理解改进现有技术所需的结构-功能关系。分离驱动所需物理过程的特定核运动和分子结构将提供一个化学蓝图，从而实现高效电子和光伏器件的合理设计与制造。从这个角度出发，我们讨论了促进FSRS用于固态样品的技术挑战和实验进展，探讨了先前确定电荷转移反应中结构-功能关系的研究，并分析了将拓宽和推动该领域发展的未来进展。
