Dataset Information

Tip-Enhanced Stokes-Anti-Stokes Scattering from Carbyne.

ABSTRACT: Carbyne, a linear chain of carbon atoms, is the truly one-dimensional allotrope of carbon and the strongest known Raman scatterer. Here, we use tip-enhanced Raman scattering (TERS) to further enhance the Raman response of a single carbyne chain confined inside a double-walled carbon nanotube. We observe an increase of the anti-Stokes scattering by a factor of 3290 and a 22-fold enhancement of the anti-Stokes/Stokes ratio relative to far-field measurements. The power dependence of the anti-Stokes/Stokes ratio under TERS conditions is indicative of coherent Stokes-anti-Stokes scattering mediated by an excited phonon. The role of resonance effects and laser-induced heating are discussed and potential opportunities are outlined.

SUBMITTER: Tschannen CD

PROVIDER: S-EPMC9052751 | biostudies-literature | 2022 Apr

REPOSITORIES: biostudies-literature

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Tip-Enhanced Stokes-Anti-Stokes Scattering from Carbyne.

Tschannen Cla Duri CD Frimmer Martin M Vasconcelos Thiago L TL Shi Lei L Pichler Thomas T Novotny Lukas L

Nano letters 20220413 8

Carbyne, a linear chain of carbon atoms, is the truly one-dimensional allotrope of carbon and the strongest known Raman scatterer. Here, we use tip-enhanced Raman scattering (TERS) to further enhance the Raman response of a single carbyne chain confined inside a double-walled carbon nanotube. We observe an increase of the anti-Stokes scattering by a factor of 3290 and a 22-fold enhancement of the anti-Stokes/Stokes ratio relative to far-field measurements. The power dependence of the anti-Stokes ...[more]

PMID: 35417179

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Project description: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.

Dataset Information

Tip-Enhanced Stokes-Anti-Stokes Scattering from Carbyne.

Publications

Tip-Enhanced Stokes-Anti-Stokes Scattering from Carbyne.

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