Dataset Information

Spatially Resolving the Enhancement Effect in Surface-Enhanced Coherent Anti-Stokes Raman Scattering by Plasmonic Doppler Gratings.

ABSTRACT: Well-designed plasmonic nanostructures can mediate far and near optical fields and thereby enhance light-matter interactions. To obtain the best overall enhancement, structural parameters need to be carefully tuned to obtain the largest enhancement at the input and output frequencies. This is, however, challenging for nonlinear light-matter interactions involving multiple frequencies because obtaining the full picture of structure-dependent enhancement at individual frequencies is not easy. In this work, we introduce the platform of plasmonic Doppler grating (PDG) to experimentally investigate the enhancement effect of plasmonic gratings in the input and output beams of nonlinear surface-enhanced coherent anti-Stokes Raman scattering (SECARS). PDGs are designable azimuthally chirped gratings that provide broadband and spatially dispersed plasmonic enhancement. Therefore, they offer the opportunity to observe and compare the overall enhancement from different combinations of enhancement in individual input and output beams. We first confirm PDG's capability of spatially separating the input and output enhancement in linear surface-enhanced fluorescence and Raman scattering. We then investigate spatially resolved enhancement in nonlinear SECARS, where coherent interaction of the pump, Stokes, and anti-Stokes beams is enhanced by the plasmonic gratings. By mapping the SECARS signal and analyzing the azimuthal angle-dependent intensity, we characterize the enhancement at individual frequencies. Together with theoretical analysis, we show that while simultaneous enhancement in the input and output beams is important for SECARS, the enhancement in the pump and anti-Stokes beams plays a more critical role in the overall enhancement than that in the Stokes beam. This work provides an insight into the enhancement mechanism of plasmon-enhanced spectroscopy, which is important for the design and optimization of plasmonic gratings. The PDG platform may also be applied to study enhancement mechanisms in other nonlinear light-matter interactions or the impact of plasmonic gratings on the fluorescence lifetime.

SUBMITTER: Ouyang L

PROVIDER: S-EPMC7944573 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Publications

Spatially Resolving the Enhancement Effect in Surface-Enhanced Coherent Anti-Stokes Raman Scattering by Plasmonic Doppler Gratings.

Ouyang Lei L Meyer-Zedler Tobias T See Kel-Meng KM Chen Wei-Liang WL Lin Fan-Cheng FC Akimov Denis D Ehtesabi Sadaf S Richter Martin M Schmitt Michael M Chang Yu-Ming YM Gräfe Stefanie S Popp Jürgen J Huang Jer-Shing JS

ACS nano 20201223 1

Well-designed plasmonic nanostructures can mediate far and near optical fields and thereby enhance light-matter interactions. To obtain the best overall enhancement, structural parameters need to be carefully tuned to obtain the largest enhancement at the input and output frequencies. This is, however, challenging for nonlinear light-matter interactions involving multiple frequencies because obtaining the full picture of structure-dependent enhancement at individual frequencies is not easy. In t ...[more]

PMID: 33356140

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Project description:Coherent Raman imaging has been extensively applied to live-cell imaging in the last 2 decades, allowing to probe the intracellular lipid, protein, nucleic acid, and water content with a high-acquisition rate and sensitivity. In this context, multiplex coherent anti-Stokes Raman scattering (MCARS) microspectroscopy using sub-nanosecond laser pulses is now recognized as a mature and straightforward technology for label-free bioimaging, offering the high spectral resolution of conventional Raman spectroscopy with reduced acquisition time. Here, we introduce the combination of the MCARS imaging technique with unsupervised data analysis based on multivariate curve resolution (MCR). The MCR process is implemented under the classical signal non-negativity constraint and, even more originally, under a new spatial constraint based on cell segmentation. We thus introduce a new methodology for hyperspectral cell imaging and segmentation, based on a simple, unsupervised workflow without any spectrum-to-spectrum phase retrieval computation. We first assess the robustness of our approach by considering cells of different types, namely, from the human HEK293 and murine C2C12 lines. To evaluate its applicability over a broader range, we then study HEK293 cells in different physiological states and experimental situations. Specifically, we compare an interphasic cell with a mitotic (prophase) one. We also present a comparison between a fixed cell and a living cell, in order to visualize the potential changes induced by the fixation protocol in cellular architecture. Next, with the aim of assessing more precisely the sensitivity of our approach, we study HEK293 living cells overexpressing tropomyosin-related kinase B (TrkB), a cancer-related membrane receptor, depending on the presence of its ligand, brain-derived neurotrophic factor (BDNF). Finally, the segmentation capability of the approach is evaluated in the case of a single cell and also by considering cell clusters of various sizes.

Dataset Information

Spatially Resolving the Enhancement Effect in Surface-Enhanced Coherent Anti-Stokes Raman Scattering by Plasmonic Doppler Gratings.

Publications

Spatially Resolving the Enhancement Effect in Surface-Enhanced Coherent Anti-Stokes Raman Scattering by Plasmonic Doppler Gratings.

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