We have developed a semianalytical theory to study a quantum plasmonic system composed of a quantum particle and a metallic particle with finite size. The quantum particle is composed of molecules driven by three laser fields and produces a coherent anti-Stokes Raman scattering (CARS) signal which is enhanced by plasmonic resonance of the metallic particle. The enhanced CARS field and the control laser form a $\mathrm{\ensuremath{\Lambda}}$ scheme that gives highly nonlinear and spatially nonlocal effects. We obtain absorption spectra that show periodic oscillations with radius of the spherical quantum particle, the whispering gallery effect. Plasmonic resonance gives very large and narrow absorption peaks as well as vanishing absorption or Fano dip at specific values of frequency and interparticle distance. The space between the two particles provides a resonant cavity effect which explains the oscillations of absorption power spectra with interparticle distance.
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.
Results from a study of quantum noise and its macroscopic manifestations in stimulated Raman scattering are presented.Shot to shot fluctuations in quantum noise initiated Stokes spectra are considered.The Stokes spectra were recorded experimentally using a Fabry-Perot interferometer.For comparison, numerically generated Stokes spectra were produced using the semi-classical model of stimulated Raman scattering with a numerically generated "vacuum" input field.The amount of structure on each spectrum was quantified by calculating the spectrum's standard deviation from its mean frequency.It was found that ensembles with the noisy spectra removed had narrower distributions of mean frequencies than ensembles that included noisy spectra.
We have studied the diffractive coupling of Stokes, anti-Stokes, and pump fields in stimulated Raman scattering. We find that, depending on the strength of the anti-Stokes field relative to that of the Stokes, both soliton dynamics and beam-pointing fluctuations are affected for finite Fresnel numbers. The generation of the anti-Stokes waves can inhibit a gain-focusing mechanism that we predicted for the Stokes field, when a soliton propagates in the medium. Although no qualitative differences arise in the beam-pointing fluctuations of the Stokes field, we predict that the anti-Stokes beam may be much more stable than the Stokes counterpart. Our analysis shows that for a Fresnel number of 5, the difference can be as large as 70%, while for Fresnel numbers of order unity, it is nearly 10%.
Coherent Raman scattering can generate Stokes and anti-Stokes fields of comparable intensities. When the Raman shift is due to a magnetic resonance transition (usually in the MHz to GHz range), the Raman fields are generally detected by optical heterodyne detection, using the excitation laser as the local oscillator. In this case, the two sidebands generate beat signals at the same frequency and are therefore indistinguishable. Separation of the two contributions becomes possible, however, by superheterodyne detection with a frequency-shifted optical local oscillator. We compare the two scattering processes, and show how the symmetry between them can be broken in
Pr3+:YAlO3.Saturation effects in coherent anti-Stokes Raman scattering (CARS) spectroscopy are discussed. The discussion is limited to Raman-resonant CARS (${\ensuremath{\omega}}_{l}\ensuremath{-}{\ensuremath{\omega}}_{s}\ensuremath{\simeq}{\ensuremath{\omega}}_{21}$, where ${\ensuremath{\omega}}_{l,s}$ are the frequencies of the pump fields with powers
Pl,s, and ${\ensuremath{\omega}}_{21}$ is the frequency of the Raman transition $|1〉\ensuremath{\rightarrow}|2〉$) with the possible addition of a one-photon resonance (${\ensuremath{\omega}}_{l}\ensuremath{\simeq}{\ensuremath{\omega}}_{31}$ is the frequency of the electronic transition $|1〉\ensuremath{\rightarrow}|3〉$). For these cases we show that the CARS polarization
pCARS is proportional to the off-diagonal density-matrix element ${\ensuremath{\rho}}_{21}$. In order to determine ${\ensuremath{\rho}}_{21}$, we use Laplace transforms to solve the Bloch equations for the effective two-level system
∣1〉 and
∣2〉 when ${\ensuremath{\omega}}_{l}$ is far from resonance, or for the three-level system
∣1〉,∣2〉, and
∣3〉, when ${\ensuremath{\omega}}_{l}\ensuremath{\simeq}{\ensuremath{\omega}}_{31}$. The steady-state expression for
pCARS in the former case gives ${\mathcal{p}}_{\mathrm{CARS}}\ensuremath{\propto}{P}_{l}{P}_{s}^{\frac{1}{2}}$ at low powers and ${\mathcal{p}}_{\mathrm{CARS}}\ensuremath{\propto}{P}_{l}^{0}{P}_{s}^{\frac{\ensuremath{-}1}{2}}$ at high powers. In the three-level system, we show that when the pressure is low and at least one field is weak, the slow time dependence of ${\ensuremath{\rho}}_{21}$ must be considered. When one field is strong and the other weak, the CARS spectrum is Stark split. When
Pl is high, for example, ${\mathcal{p}}_{\mathrm{CARS}}\ensuremath{\propto}{P}_{l}^{0}{P}_{s}^{\frac{1}{2}}$ for ${\ensuremath{\omega}}_{s}\ensuremath{\simeq}{\ensuremath{\omega}}_{32}$ and ${\mathcal{p}}_{\mathrm{CARS}}\ensuremath{\propto}{({P}_{l}{P}_{s})}^{\frac{1}{2}}$ when ${\ensuremath{\omega}}_{s}\ensuremath{\simeq}{\ensuremath{\omega}}_{32}\ifmmode\pm\else\textpm\fi{}{V}_{13}$ where
V13 is the one-photon Rabi frequency for the $|1〉\ensuremath{\rightarrow}|3〉$ transition. The Wilcox-Lamb approximation is used to reduce the three-level Bloch equations to rate equations containing one- and two-photon terms. When the fields are so weak that both one- and two-photon terms are small compared to the decay terms, the usual expression for
pCARS is reproduced. If only the direct two-photon processes are important, the effective-two-system results are reproduced. When both fields are intense and nearly resonant, the steady state is rapidly achieved. The results for the case where one field is much stronger than the other are essentially the same as those for one strong and one weak field. When the fields are of comparable strength, ${\mathcal{p}}_{\mathrm{CARS}}\ensuremath{\propto}{P}_{l}^{\frac{1}{2}}{P}_{s}^{0}$ for ${\ensuremath{\omega}}_{l}\ensuremath{\simeq}{\ensuremath{\omega}}_{31}$ and ${\ensuremath{\omega}}_{s}\ensuremath{\simeq}{\ensuremath{\omega}}_{32}$, and the CARS spectrum is split into five components.