A unified framework for the description of plasmonically enhanced ultrafast and cw Raman spectroscopies

L. D. Ziegler

doi:10.1117/12.2676824

3 October 2023 A unified framework for the description of plasmonically enhanced ultrafast and cw Raman spectroscopies

L. D. Ziegler

Proceedings Volume 12654, Enhanced Spectroscopies and Nanoimaging 2023; 1265405 (2023) https://doi.org/10.1117/12.2676824
Event: SPIE Nanoscience + Engineering, 2023, San Diego, California, United States

Abstract

Spontaneous and stimulated Raman spectroscopies provide label-free, diffraction and sub-diffraction limited imaging capabilities, particularly valuable for biomedical applications. Plasmonically enhanced (PE) nonlinear versions of these spectroscopies can potentially provide even higher sensitivities enabling more rapid chemical imaging of a wider range of analytes for “real time” applications. A unifying density matrix framework for treating all plasmon-enhanced molecular spectroscopies is presented. The temporal description of PE optical electric fields of any pulse duration is an essential first step. The effects of the complex plasmonic enhancement factor on ultrafast, picosecond and cw pulses based on an idealized Lorentz oscillator model and observed dielectric properties of metal nanoparticle structures is shown. In particular, plasmonic enhancement effects on the optical phase, carrier frequency and pulse duration of incident ultrafast pulses are described. Unlike spontaneous PE Raman (SERS), the locally generated signal field of plasmon-enhanced stimulated Raman spectroscopies is also itself enhanced by a plasmonic response. A density matrix framework formulism is used to describe plasmonically enhanced femtosecond stimulated Raman scattering (FSRS), stimulated Raman gain/loss (SRG/L), impulsive stimulated Raman, CARS and spontaneous Raman. Plasmonic enhanced ultrafast pulses result in Raman spectroscopies that display dispersive vibrational line shapes (FSRS) or mixed dichroic and birefringent nuclear coherences (pump-probe) in agreement with experimental observations.

Conference Presentation

(2023) Published by SPIE. Downloading of the abstract is permitted for personal use only.

Citation Download Citation

L. D. Ziegler "A unified framework for the description of plasmonically enhanced ultrafast and cw Raman spectroscopies", Proc. SPIE 12654, Enhanced Spectroscopies and Nanoimaging 2023, 1265405 (3 October 2023); https://doi.org/10.1117/12.2676824

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