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The mechanism of formation of the polarimetric signal observed in the spin noise spectroscopy (SNS) is analyzed from the viewpoint of the light scattering theory. A rigorous calculation of the polarimetric signal (Faraday rotation or ellipticity) recorded in the SNS is presented in the approximation of single scattering. We show that it is most correctly to consider this noise as a result of scattering of the probe light beam by fluctuating susceptibility of the medium. Fluctuations of the gyrotropic (antisymmetric) part of the susceptibility tensor lead to appearance of the typical for the SNS Faraday rotation noise at the Larmor frequency. At the same time, fluctuations of linear anisotropy of the medium (symmetric part of the susceptibility tensor) give rise to the ellipticity noise of the probe beam spectrally localized at the double Larmor frequency. The results of the theoretical analysis well agree with the experimental data on the ellipticity noise in cesium vapor.
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The Dipole-Quadrupole theory of Surface Enhanced Hyper Raman Scattering (SEHRS), created by the authors is expounded in details. Peculiarities of the behavior of electromagnetic field on rough metal surfaces are considered. It is demonstrated that there is an enhancement of the dipole and quadrupole light-molecule interaction near the places with a large curvature. The expression for the SEHRS cross-section of symmetrical molecules, which consists of several contributions is obtained. Selection rules for the scattering contributions are obtained and a qualitative classification of the contributions after an enhancement degree is performed. Analysis of experimental spectra of pyrazine and phenazine, and also some another molecules is performed too. It is demonstrated a full coincidence of experimental regularities in these spectra with the theory suggested.
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.
Ramsey interferometry provides a natural way to determine the coherence time of most qubit systems. Recent experiments on quantum dots however, demonstrated that dynamical nuclear spin polarization can strongly influence the measurement process, making it difficult to extract the $T_2^*$ coherence time using optical Ramsey pulses. Here, we demonstrate an alternative method for spin coherence measurement that is based on first-order coherence of photons generated in spin-flip Raman scattering. We show that if a quantum emitter is driven by a weak monochromatic laser, Raman coherence is determined exclusively by spin coherence, allowing for a direct determination of spin $T_2^*$ time. When combined with coherence measurements on Rayleigh scattered photons, our technique enables us to identify coherent and incoherent contributions to resonance fluorescence, and to minimize the latter. We verify the validity of our technique by comparing our results to those determined from Ramsey interferometry for electron and heavy-hole spins.
Revealing hidden non-radiative (dark) of resonant nanostructures using optical methods such as dark-field spectroscopy often becomes a sophisticated problem due to a weak coupling of these modes with a far-field radiation, whereas methods of dark-modes spectroscopy, e.g. cathodoluminescence or elastic energy losses, are not always convenient in use. Here, we suggest an approach for experimental determining the mode structure of a nanoresonator basing on utilizing intrinsic incoherent Raman scattering. We theoretically predict the efficiency of this approach and realize it experimentally for silicon nanoparticle resonators possessing strong Raman line at 520 cm^-1. With this method, we studied a silicon nanoparticle placed on a gold substrate and reveal the spectral position of a low-radiative magnetic quadrupole mode which is hardly observable with common dark-field optical spectroscopy.
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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