Surface-enhanced femtosecond stimulated Raman scattering (SE-FSRS) is one form of surface-enhanced coherent Raman scattering (SECRS) techniques that are ideally suited for observing the molecule-plasmon interactions involved in chemical change driven or enhanced by plasmonic nanomaterials. As plasmonic nanomaterials have seen diverse uses from optical nanoantennas to chemical nanoreactors, further developing techniques that can both initiate and track these chemical changes, like SE-FSRS is highly important. To this end, we have developed a variety of tools to further the use of SE-FSRS as an analytical technique. In this talk I will discuss our recent work in developing classical and quantum mechanical theories of SE-FSRS, experimental progress in improving SE-FSRS spectrometers, as well as new experiments showing stimulated Raman loss (SRL) in SE-FSRS and single-aggregate SE-FSRS. An important aspect of this work is the continual back-and-forth theory-experiment collaboration that has allowed for continual improvement in the SE-FSRS technique. The classical theory of SE-FSRS explained initial results well, but pushing the experimental techniques further resulted in the need for the quantum mechanical theory of SE-FSRS. Similarly, the quantum mechanical theory of SE-FSRS drove the need for attaining single-aggregate SE-FSRS experimentally. Further developing SE-FSRS experimentally and theoretically will allow for an improved analytical technique that can probe coupled molecule-plasmon interactions, potentially leading to a SECRS spectroscopy that can be used for initiating and tracking plasmonic chemistry.

Understanding molecule-plasmon coupling in surface-enhanced femtosecond stimulated Raman scattering: Combined experimental-theoretical studies

253rd National Meeting (2017)

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