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Register a new userQED description of Raman scattering from molecules in plasmonic cavities
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Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of textit{phonon-stimulated Raman scattering} and an counter-intuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this novel QED framework opens a venue to analyze the correlations of photons emitted at a plasmonic cavity
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The differential response of chiral molecules to incident left- and right- handed circularly polarized light is used for sensing the handedness of molecules. Currently, significant effort is directed towards enhancing weak differential signals from the molecules, with the goal of extending the capabilities of chiral spectrometers to lower molecular concentrations or small analyte volumes. Previously, optical cavities for enhancing vibrational circular dichroism have been introduced. Their enhancements are mediated by helicity-preserving cavity modes which maintain the handedness of light due to their degenerate TE and TM components. In this article, we simplify the design of the cavity, and numerically compare it with the previous one using an improved model for the response of chiral molecules. We use parameters of molecular resonances to show that the cavities are capable of bringing the vibrational circular dichroism signal over the detection threshold of typical spectrometers for concentrations that are one to three orders of magnitude smaller than those needed without the cavities, for a fixed analyte volume. Frequency resolutions of current spectrometers result in enhancements of more than one order (two orders) of magnitude for the new (previous) design. With improved frequency resolution, the new design achieves enhancements of three orders of magnitude. We show that the TE/TM degeneracy in perfectly helicity preserving modes is lifted by factors that are inherent to the cavities. More surprisingly, this degeneracy is also lifted by the molecules themselves due to their lack of electromagnetic duality symmetry, that is, due to the partial change of helicity during the light-molecule interactions.
Orbital angular momentum of light is a core feature in photonics. Its confinement to surfaces using plasmonics has unlocked many phenomena and potential applications. Here we introduce the reflection from structural boundaries as a new degree of freedom to generate and control plasmonic orbital angular momentum. We experimentally demonstrate plasmonic vortex cavities, generating a succession of vortex pulses with increasing topological charge as a function of time. We track the spatio-temporal dynamics of these angularly decelerating plasmon pulse train within the cavities for over 300 femtoseconds using time-resolved Photoemission Electron Microscopy, showing that the angular momentum grows by multiples of the chiral order of the cavity. The introduction of this degree of freedom to tame orbital angular momentum delivered by plasmonic vortices, could miniaturize pump-probe-like quantum initialization schemes, increase the torque exerted by plasmonic tweezers and potentially achieve vortex lattice cavities with dynamically evolving topology.
We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multi-plasmon/photon Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission. To illustrate the practical application of the theory, we show examples using a gold nanorod dimer and a hybrid dielectric-metal cavity structure.
We present a theoretical study of the optical angular momentum transfer from a circularly polarized plane wave to thin metal nanoparticles of different rotational symmetries. While absorption has been regarded as the predominant mechanism of torque generation on the nanoscale, we demonstrate numerically how the contribution from scattering can be enhanced by using multipolar plasmon resonance. The multipolar modes in non-circular particles can convert the angular momentum carried by the scattered field, thereby producing scattering-dominant optical torque, while a circularly symmetric particle cannot. Our results show that the optical torque induced by resonant scattering can contribute to 80% of the total optical torque in gold particles. This scattering-dominant torque generation is extremely mode-specific, and deserves to be distinguished from the absorption-dominant mechanism. Our findings might have applications in optical manipulation on the nanoscale as well as new designs in plasmonics and metamaterials.
Stimulated Raman scattering is a well-known nonlinear process that can be harnessed to produce optical gain in a wide variety of media. This effect has been used to produce the first silicon-based lasers and high-gain amplifiers. Interestingly, the Raman effect can also produce intensity-dependent nonlinear loss through a corollary process known as inverse Raman scattering (IRS). Here, we demonstrate IRS in silicon--a process that is substantially modified by the presence of optically-generated free carriers--achieving attenuation levels >15 dB with a pump intensity of 4 GW/cm^2. Ironically, we find that free-carrier absorption, the detrimental effect that suppresses other nonlinear effects in silicon, actually facilitates IRS by delaying the onset of contamination from coherent anti-Stokes Raman scattering. The carriers allow significant IRS attenuation over a wide intensity range. Silicon-based IRS could be used to produce chip-scale wavelength-division multiplexers, optical signal inverters, and fast optical switches.
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