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Physical Review A

Enhancement of nonclassical Raman light intensity by plasmonic nanoantenna

Vladislav Yu. Shishkov, E. S. Andrianov, Alexander Pukhov, Alexey P. Vinogradov

Published Jan 26, 2021• 3 citations
Publisher

Abstract

As is well known, light arising from Raman scattering on molecules shows nonclassical mutual correlations between the Stokes and anti-Stokes components. However, the practical use of nonclassical Raman light is limited, due to its low intensity. The Raman signal can be enhanced in surface-enhanced Raman scattering (SERS) experiments by placing Raman active molecules near a plasmonic nanoantenna, due to the Purcell effect. Since the main contribution to emission in SERS experiments is re-emitted light from the plasmonic nanoantenna with no nonclassical correlations, the question arises as to whether it is possible to simultaneously amplify the Raman signal and preserve the nonclassical correlations. In this work, we give a positive answer to this question. We show that plasmonic nanoantennas can be used to enhance the nonclassical light intensity. We demonstrate that the main factor causing deterioration of the cross correlations of SERS light is the fluorescent background of the plasmonic nanoantenna. We analyze the way in which the geometry of a plasmonic nanoantenna affects the nonclassical cross correlations of the Raman light, and show that there is an optimal size of plasmonic nanoantenna that both increases the Raman signal and preserves the nonclassical correlations of the light at the level of a single molecule. The obtained results pave the way for the creation of sources with controlled intensity and a degree of nonclassicality.

DOI
10.1103/physreva.103.013725

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As is well known, light arising from Raman scattering on molecules shows nonclassical mutual correlations between the Stokes and anti-Stokes components. However, the practical use of nonclassical Raman light is limited, due to its low intensity. The Raman signal can be enhanced in surface-enhanced Raman scattering (SERS) experiments by placing Raman active molecules near a plasmonic nanoantenna, due to the Purcell effect. Since the main contribution to emission in SERS experiments is re-emitted light from the plasmonic nanoantenna with no nonclassical correlations, the question arises as to whether it is possible to simultaneously amplify the Raman signal and preserve the nonclassical correlations. In this work, we give a positive answer to this question. We show that plasmonic nanoantennas can be used to enhance the nonclassical light intensity. We demonstrate that the main factor causing deterioration of the cross correlations of SERS light is the fluorescent background of the plasmonic nanoantenna. We analyze the way in which the geometry of a plasmonic nanoantenna affects the nonclassical cross correlations of the Raman light, and show that there is an optimal size of plasmonic nanoantenna that both increases the Raman signal and preserves the nonclassical correlations of the light at the level of a single molecule. The obtained results pave the way for the creation of sources with controlled intensity and a degree of nonclassicality.
In the context of the quantum-mechanical description of single-molecule surface-enhanced Raman scattering, intensity-field correlation measurements of photons emitted from a plasmonic cavity are explored, theoretically, using the technique of conditional homodyne detection. The inelastic interplay between plasmons and vibrations of a diatomic molecule placed inside the cavity can be manifested in phase-dependent third-order fluctuations of the light recorded by the aforesaid technique, allowing us to reveal signatures of non-classicality (indicatives of squeezing) of the outgoing Raman photons.
It is known that spontaneous Raman scattering is accompanied by the appearance of nonclassical cross correlations of photons at Stokes and anti-Stokes frequencies. Such correlations occur due to the internal nonlinear interaction between electronic and nuclear vibration degrees of freedom. Since the properties of a given media are unchangeable, the possibilities for controlling the cross correlations are limited. This, in turn, restricts the possible applications of the correlated light obtained during the spontaneous Raman scattering. In this work, we investigate the influence of statistical properties of an incident light on the cross correlations of Stokes and anti-Stokes light. We show that the incoherence of the incident light results not only in the incoherence of the scattered light but also in the enhancement of the interbeam coherence at different frequencies. We demonstrate that the cross correlations of Stokes and anti-Stokes light intensities are enhanced when the incident light with high second-order autocorrelation function is applied. Our results pave the way to control correlated light obtained in the process of spontaneous Raman scattering.
We identify enhanced strong coherent Surface-Enhanced Raman Scattering (SERS) interactions facilitated by hybridized metallo-dielectric cavities with a resonant fluorescent molecule. By illuminating a detuned electronic transition near saturation via a narrowband hybrid plasmonic mode, we observe enhanced splittings in the Stokes and anti-Stokes spectra, revealing strong optomechanical coupling and nonlinear vibrational modifications at intensities far below irreversible SERS damage thresholds. We compute the second-order photon correlations that allows identifying the nonclassical character associated to these strong optomechanical interactions and SERS configurations that enables them to optically characterize the anharmonic character of the vibrational modes.
We study Raman scattering in active media placed in proximity of different types of metal nanostructures, at wavelengths that display either Fabry-Perot or plasmonic resonances, or a combination of both. We use a semi-classical approach to derive equations of motion for Stokes and anti-Stokes fields that arise from quantum fluctuations. Our calculations suggest that local field enhancement yields Stokes and anti-Stokes conversion efficiencies between five and seven orders of magnitudes larger compared to cases without the metal nanostructure. We also show that to first order in the linear susceptibility the local field correction induces a dynamic, intensity-dependent frequency detuning that at high intensities tends to quench Raman gain.
Light with high mutual correlations at different frequencies can be used to create heralded single-photon sources, which may serve as the basic elements of existing quantum cryptography and quantum teleportation schemes. One of the important examples in natural systems of light with high mutual correlations is the light produced by spontaneous Raman scattering on an ensemble of molecules. In this paper, we investigate the possibility of using Raman light to create a heralded single-photon source. We show that when using Stokes scattered light for postselection of anti-Stokes scattered light, the latter may possess single-photon properties. We analyze the influence of various negative factors on the characteristics of such a heralded single-photon source, which include a time delay between Stokes and anti-Stokes photons, the finiteness of the correlation radius of an external source, and background radiation. We show that the low value of the second-order autocorrelation function of the single-photon source is preserved even when the flow of uncorrelated photons exceeds the flow of correlated photons in scattered Raman light by an order of magnitude.
Quantum electrodynamics theory of the resonance Raman scattering is developed for an atom in a close proximity to a carbon nanotube. The theory predicts a dramatic enhancement of the Raman intensity in the strong atomic coupling regime to nanotube plasmon near-fields. This resonance scattering is a manifestation of the general electromagnetic surface enhanced Raman scattering effect, and can be used in designing efficient nanotube based optical sensing substrates for single atom detection, precision spontaneous emission control, and manipulation.