From SERS to TERS and Beyond: Molecules as Probes of Nanoscopic Optical Fields.
From SERS to TERS and Beyond: Molecules as Probes of Nanoscopic Optical Fields.
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DOI：
10.1021/acs.jpcc.0c08337
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发表时间：
2020-12-17
期刊：
影响因子：
--
通讯作者：
Schultz ZD
中科院分区：
文献类型：
--
作者：
El-Khoury PZ;Schultz ZD
详细了解分子和等离子体纳米结构之间的相互作用对于（生物）分子传感和成像，催化以及能量转换中的几个令人兴奋的发展非常重要。虽然大部分的焦点一直在纳米结构，产生增强和纳米限制的光场，我们在这里强调最近的工作，从我们的小组，使用表面和尖端增强拉曼散射（Sers和TERS，分别）的分子响应，调查不同方面的本地字段。TERS提供了对超受限体积的访问，因此可以进一步探索和解释整体平均Sers测量。在等离子体激元的量子极限下，观察到了激发的和独特的分子行为，包括分子充电、化学转化和光整流。来自分子的多极拉曼散射的证据还提供了对驱动Sers和TERS的不均匀电场及其空间和时间梯度的见解。这些过程的时间尺度显示出合作的纳米级现象，共同有助于Sers和TERS的证据。
A detailed understanding of the interaction between molecules and plasmonic nanostructures is important for several exciting developments in (bio)molecular sensing and imaging, catalysis, as well as energy conversion. While much of the focus has been on the nanostructures that generate enhanced and nano-confined optical fields, we herein highlight recent work from our groups that uses the molecular response in surface and tip enhanced Raman scattering (SERS and TERS, respectively) to investigate different aspects of the local fields. TERS provides access to ultra-confined volumes, and as a result can further explore and explain ensemble-averaged SERS measurements. Exciting and distinct molecular behaviors are observed in the quantum limit of plasmons, including molecular charging, chemical conversion, and optical rectification. Evidence of multipolar Raman scattering from molecules additionally provides insights into the inhomogeneous electric fields that drive SERS and TERS and their spatial and temporal gradients. The time scales of these processes show evidence of cooperative nanoscale phenomena that altogether contribute to SERS and TERS.
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