The interaction between two metallic spheres with radius R with external electromagnetic (EM) field polarized in the symmetric z direction is described. Solutions of Laplace equation with bi-spherical coordinates are developed. Hot spots are obtained under the condition that the shortest distance between the two spheres surfaces is very small relative to their radius. Boundary conditions are applied which assume very large real negative value for the dielectric constant of the metallic spheres which is valid for atoms like that of AG or Au at certain frequencies. Under these conditions the EM field is amplified by many orders of magnitudes relative to the incident EM field. Analytical results for maximal Raman enhancement factor (EF ) are obtained as function of various parameters. The present study can be applied to surface-enhanced Raman spectroscopy (SERS) and two-photon induced illumination (TPI-PL) in which the amplification is proportional to the fourth power of the incident EM field.
Plasmonic nanostructures enhance nonlinear response, such as surface enhanced Raman scattering (SERS), by localizing the incident field into hot spots. The localized hot spot field can be enhanced even further when linear Fano resonances (FR) take place in a double resonance scheme. However, hot spot enhancement is limited with the modification of the vibrational modes, the break-down of the molecule and the tunnelling regime. Here, we present a method which can circumvent these limitations. Our analytical model and solutions of 3D Maxwell equations show that: enhancement due to the localized …
Molecular optomechanics stems from the description of Raman scattering in the presence of an optical resonator using a cavity optomechanics formalism. We extend the molecular optomechanics formalism to the case of hybrid dielectric-plasmonic resonators, with multiple optical resonances and with both free-space and waveguide addressing. We demonstrate how the Raman enhancement is the product of a pump enhancement and a modified LDOS, that simply depend on the complex response functions of the hybrid system. The Fano lineshapes that result from hybridization of a broadband and narrowband modes a…
Raman scattering signal can be enhanced through localization of incident field into sub-wavelength hot-spots through plasmonic nano-structures (Surface-enhanced Raman scattering-SERS). Recently, further enhancement of SERS signal via quantum objects are proposed by [1] without increasing the hot-spot intensity (\textit{silent-enhancement}) where this suggestion prevents the modification of vibrational modes or the breakdown of molecules. The method utilizes path interference in the non-linear response of Stokes-shifted Raman modes. In this work, we extend this phenomenon to tune the spectral p…
Surface-enhanced coherent anti-Stokes Raman scattering (SE-CARS) takes advantage of surface plasmon resonances supported on metallic nanostructures to amplify the coherent Raman response of target molecules. While these metallic antennas have found significant success in SE-CARS studies, photo-induced morphological changes to the nanoantenna under ultrafast excitation introduce significant hurdles in terms of stability and reproducilibty. These hurdles need to be overcome in order to establish SE-CARS as a reliable tool for rapid biomolecular sensing. Here we address this challenge by performi…
Detection of enantiomers is a challenging problem in drug development as well as environmental and food quality monitoring where traditional optical detection methods suffer from low signals and sensitivity. Application of surface enhanced Raman scattering (SERS) for enantiomeric discrimination is a powerful approach for the analysis of optically active small organic or large biomolecules. In this work, for enantio-selective sensing we proposed the coupling of disposable chiral plasmonic shurikens supporting the chiral near-field distribution with SERS active silver nanoclusters. As a result o…
We show that topology optimization (TO) of metallic resonators can lead to $\sim 10^2\times$ improvement in surface-enhanced Raman scattering (SERS) efficiency compared to traditional resonant structures such as bowtie antennas. TO inverse design leads to surprising structures very different from conventional designs, which simultaneously optimize focusing of the incident wave and emission from the Raman dipole. We consider isolated metallic particles as well as more complicated configurations such as periodic surfaces or resonators coupled to dielectric waveguides, and the benefits of TO are …
Investigating Analyte Co-Localization at Electromagnetic Gap Hot-Spots For Highly Sensitive (Bio)molecular Detection by Plasmon Enhanced Spectroscopies
Topology-optimized distributed 3d anisotropic Raman emission
Massachusetts Institute of Technology（麻省理工学院）；Vrije Universiteit Amsterdam（阿姆斯特丹自由大学）；Rice University（莱斯大学）；Duke University（杜克大学）；Technical University of Denmark（丹麦技术大学）
The Raman scattering of light by molecular vibrations offers a powerful technique to 'fingerprint' molecules via their internal bonds and symmetries. Since Raman scattering is weak, methods to enhance, direct and harness it are highly desirable, e.g. through the use of optical cavities, waveguides, and surface enhanced Raman scattering (SERS). While SERS offers dramatic enhancements by localizing light within vanishingly small 'hot-spots' in metallic nanostructures, these tiny interaction volumes are only sensitive to few molecules, yielding weak signals that are difficult to detect. Here, we …
The theoretical method to study strong coupling between an ensemble of quantum emitters (QEs) and surface plasmons excited by the nanoparticle cluster has been presented by using a rigorous first-principles electromagnetic Green's tensor technique. We have demonstrated that multi-qubit entanglement for two-level QEs can be produced at different frequencies simultaneously, when they locate in hot spots of metallic nanoparticle clusters. The duration of quantum beats for such an entanglement can reach two orders longer than that for the entanglement in a photonic cavity. The phenomenon originate…
To develop highly sensitive, stable and repeatable surface-enhanced Raman scattering (SERS) substrates is crucial for analytical detection, which is a challenge for traditional metallic structures. Herein, by taking advantage of the high surface activity of 1T' transition metal telluride, we have fabricated high-density gold nanoparticles (AuNPs) that are spontaneously in-situ prepared on the 1T' MoTe2 atomic layers via a facile method, forming a plasmonic-2D material hybrid SERS substrate. This AuNP formation is unique to the 1T' phase, which is repressed in 2H MoTe2 with less surface activit…
