Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
Chem Soc Rev. 2016 Apr 21;45(8):2263-90. doi: 10.1039/c5cs00763a. Epub 2016 Feb 5.
Ultrafast surface-enhanced Raman spectroscopy (SERS) has the potential to study molecular dynamics near plasmonic surfaces to better understand plasmon-mediated chemical reactions such as plasmonically-enhanced photocatalytic or photovoltaic processes. This review discusses the combination of ultrafast Raman spectroscopic techniques with plasmonic substrates for high temporal resolution, high sensitivity, and high spatial resolution vibrational spectroscopy. First, we introduce background information relevant to ultrafast SERS: the mechanisms of surface enhancement in Raman scattering, the characterization of plasmonic materials with ultrafast techniques, and early complementary techniques to study molecule-plasmon interactions. We then discuss recent advances in surface-enhanced Raman spectroscopies with ultrafast pulses with a focus on the study of molecule-plasmon coupling and molecular dynamics with high sensitivity. We also highlight the challenges faced by this field by the potential damage caused by concentrated, highly energetic pulsed fields in plasmonic hotspots, and finally the potential for future ultrafast SERS studies.
超快表面增强拉曼光谱（SERS）有可能研究等离子体表面附近的分子动力学，以更好地理解等离子体介导的化学反应，如等离子体增强光催化或光电过程。本综述讨论了将超快拉曼光谱技术与等离子体基底相结合，以实现高时间分辨率、高灵敏度和高空间分辨率振动光谱的方法。首先，我们介绍了与超快 SERS 相关的背景信息：拉曼散射中表面增强的机制、用超快技术表征等离子体材料，以及早期用于研究分子-等离子体相互作用的互补技术。然后，我们讨论了最近在超快脉冲表面增强拉曼光谱方面的进展，重点是研究分子-等离子体耦合和具有高灵敏度的分子动力学。我们还强调了该领域面临的挑战，即等离子体热点中集中的、高能量的脉冲场可能造成的潜在破坏，最后还展望了未来超快 SERS 研究的可能性。
