Hyper‐Raman Spectroscopy

Ziegler, L. D.

doi:10.1002/0470027320.s0412

Cited by 10 publications

(11 citation statements)

References 87 publications

(2 reference statements)

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“…Since it was discovered, HRS effect has aroused great interests due to its special selection rule 3 . However, HRS is a two-photon process and has a tiny scattering cross-section of about 10 –6 of NRS, so the experimental testing was very difficult 4 . It was not until the discovery of surface-enhanced Raman scattering (SERS) phenomenon that HRS was considered as an applied spectroscopy technique.…”

Section: Introductionmentioning

confidence: 99%

Plasmon coupling nanorice trimer for ultrahigh enhancement of hyper-Raman scattering

Zhu

Chen

Liang

et al. 2021

Sci Rep

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A new tactic that using Ag nanorice trimer as surface-enhanced hyper Raman scattering substrate is proposed for realizing maximum signal enhancement. In this paper, we numerically simulate and theoretically analyze the optical properties of the nanorice trimer consisting of two short nanorices and a long nanorice. The Ag nanorice trimer can excite Fano resonance at optical frequencies based on the strong interaction between the bright and the dark mode. The bright mode is attributed to the first longitudinal resonance of the short nanorice pair, while the dark mode originates from the third longitudinal mode resonance of the long nanorice. The electric field distributions demonstrate that the two resonances with the largest field strength correspond to the first-order resonance of the long nanorice and the Fano resonance of the trimer, respectively. Two plasmon resonances with maximum electromagnetic field enhancements and same spatial hot spot regions can match spectrally with the pump and second-order Stokes beams of hyper Raman scattering, respectively, through reasonable design of the trimer structure parameters. The estimated enhancement factor of surface-enhanced hyper Raman scattering can achieve as high as 5.32 × 1013.

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Section: Introductionmentioning

confidence: 99%

Plasmon coupling nanorice trimer for ultrahigh enhancement of hyper-Raman scattering

Zhu

Chen

Liang

et al. 2021

Sci Rep

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“…However, due to the two-photon process and the little cross-sections of about 10 6 times weaker than RS, the experimental detection for HRS is very difficult 5 . For a long time in the past, HRS has not been considered as an applied spectroscopic technique until people discovered surface enhancement Raman scattering (SERS) phenomenon.…”

Section: Introductionmentioning

confidence: 99%

Theoretical investigation of a plasmonic substrate with multi-resonance for surface enhanced hyper-Raman scattering

Zhu

Chen

Ding

et al. 2018

Sci Rep

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Because of the unique selection rule, hyper-Raman scattering (HRS) can provide spectral information that linear Raman and infrared spectroscopy cannot obtain. However, the weak signal is the key bottleneck that restricts the application of HRS technique in study of the molecular structure, surface or interface behavior. Here, we theoretically design and investigate a kind of plasmonic substrate consisting of Ag nanorices for enhancing the HRS signal based on the electromagnetic enhancement mechanism. The Ag nanorice can excite multiple resonances at optical and near-infrared frequencies. By properly designing the structure parameters of Ag nanorice, multi- plasmon resonances with large electromagnetic field enhancements can be excited, when the “hot spots” locate on the same spatial positions and the resonance wavelengths match with the pump and the second-order Stokes beams, respectively. Assisted by the field enhancements resulting from the first- and second-longitudinal plasmon resonance of Ag nanorice, the enhancement factor of surface enhanced hyper-Raman scattering can reach as high as 5.08 × 109, meaning 9 orders of magnitude enhancement over the conventional HRS without the plasmonic substrate.

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“…Unfortunately, the specific molecular information provided by HRS cannot be exploited without any plasmon enhancement, because the HRS signal from a single molecule is several orders of magnitude weaker than the RS signal . For example, the ratio between HRS and RS has been estimated to be 5 × 10 –9 for bulk crystal violet molecules at a laser power of 10 7 W/cm 2 . − However, the important criteria for making a good plasmonic substrate for surface-enhanced hyper-Raman scattering (SEHRS) have not been discussed in detail as was done in the past for SERS and SIERA. , The development of such an efficient substrate can unleash the potential of SEHRS, down to the single molecule sensitivity …”

Section: Introductionmentioning

confidence: 99%

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

Butet

Martin

2015

J. Phys. Chem. C

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The plasmon enhancement of molecular hyperRaman scattering, the nonlinear counterpart of Raman scattering, which involves the absorption of two fundamental photons, is investigated with emphasis on low energy molecular vibrations. The two-photon excitation of the molecule is treated using its hyperpolarizability β, and the emission of the hyperRaman photons is computed using a dipole emitter located at the molecule position. The electromagnetic response of the plasmonic systems is evaluated using a surface integral equation method, which makes possible considering both planewave and dipole excitations in a single formalism. Taking into account different geometries (including multiresonant antennas and silver heptamers supporting Fano resonances), the experimental parameters influencing the enhancement of the molecular hyperRaman scattering are discussed in detail. In particular, it is shown that a good excitation at the fundamental stage is not sufficient for reaching a good enhancement factor and that an optimization of the electromagnetic response of the plasmonic substrate is also important at the emission wavelength. The competition between the molecular hyper-Raman scattering signal and the background signal, that is, the second harmonic generation, is discussed. The latter can be reduced in specific structures by taking advantages of the key role played by the symmetry of the structure for hyper-Raman scattering and second harmonic generation. This way, we propose a nanostructure where the second harmonic generation can be reduced in the detection direction, enabling the hyper-Raman scattering signal from single donor−acceptor "push−pull" chromophores to be experimentally recorded with a low noise level using surface-enhanced hyper-Raman scattering. It is particularly remarkable that the hyper-Raman signal from one molecule can be stronger than the second harmonic generation from a complete plasmonic nanostructure, despite the considerable volume difference between both nano-objects. This fundamental observation stems from the different selection rules for both nonlinear optical processes.

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Hyper‐Raman Spectroscopy

Cited by 10 publications

References 87 publications

Plasmon coupling nanorice trimer for ultrahigh enhancement of hyper-Raman scattering

Plasmon coupling nanorice trimer for ultrahigh enhancement of hyper-Raman scattering

Theoretical investigation of a plasmonic substrate with multi-resonance for surface enhanced hyper-Raman scattering

Surface-Enhanced Hyper-Raman Scattering: A New Road to the Observation of Low Energy Molecular Vibrations

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