We report the observation of Zeno switching through an inverse Raman scattering (IRS) process in an optical fiber. In IRS, light at the anti-Stokes frequency is strongly attenuated in the presence of a pump field, allowing it to be used for all-optical switching and modulation. Our observed level of induced absorption via IRS in the optical fiber is > 20 dB in a time scale of less than 5 ps. The full Raman response spectrum was extracted experimentally and excellent agreement was found between the experimental data and theoretical modeling of IRS.
The Raman effect is the inelastic scattering of photons by matter. When a monochromatic light beam (pump beam) propagates in an optical fibre, spon- taneous Raman scattering transfers some of the photons to new frequencies. The probability of a photon scattering to a particular frequency shift, depends on that frequency shift, forming a characteristic spectrum. The scattered photons may lose energy (Stokes) or gain energy (anti-Stokes). If the pump beam is linearly polarized, then the polarization of scattered photons may be the same (parallel scattering) or orthogonal (perpendicular scattering). If photons are already present at other frequencies then the probability of scattering to those frequencies is enhanced (stimulated scattering). In this thesis, the equations governing the Raman effect, both in bulk glass and single mode fibre, are restated. The probability of spontaneous scattering (parallel and perpendicular) in an optical fibre has been measured for frequency shifts between 4THz and 58THz. Particular attention has been given to those frequency shifts where the scattering is intrinsically weak. This has identified those frequency shifts where it might be possible to eliminate Raman noise from experiments designed to generate quantum states of light in optical fibres using four wave mixing. From the measured scattering probabilities, the Raman equations can be used to predict the scattering cross-section in bulk glass. The prediction is found to be in reasonable agreement with measurements of the bulk glass cross-section published by other authors. By increasing the pump power, the transition to stimulated scattering has been observed. In the case of Stokes scattering there is reasonable agreement between the Raman equations and experimental observations. In the case of anti-Stokes scattering, and in the limit of very high pump power, behaviour is observed which is not predicted by the Raman equations, indicating that other processes must be included to successfully describe such experiments.
The theory of coherent anti-Stokes Raman scattering (CARS) is extended to include the effect of pump fluctuations. The intensities and spectra of lines in resonant CARS are calculated to all orders in fields assuming a phase-diffusion model for waves at the two pump frequencies. The bandwidth of the two lasers enters in a much more complicated way than following a simple scaling of
T1 or
T2. Various resonances in CARS spectra due to dynamic splitting of the energy levels are discussed for a range of detunings, field intensities, and bandwidths. In contrast to the usual spectra in strong fields, the Rabi sidebands appear as dispersion-shaped structures. The laser linewidth is shown to change dramatically the CARS line shape. The case of no saturation is also treated, thus allowing for the inclusion of more general line shapes and fluctuations of the pump waves and the nonlinear susceptibility tensor ${\ensuremath{\chi}}^{(3)}$. Gaussian statistics of the pump field are shown to lead to enhancement factors in CARS intensity, similar to those appearing in the context of multiphoton absorption processes.
The optical mixing of sufficiently coherent radiations of frequency (omega) 1 and (omega) 2 inside a suitable molecular medium can result coherent radiation at new frequency (omega) 3 equals [(omega) 1 + ((omega) 1 - (omega) 2)]. If (omega) 1 is kept fixed and (omega) 2 is varied so that a condition (omega) 1 - (omega) 2 equals (omega) is reached where (omega) is a molecular frequency of the medium, then (omega) 3 equals (omega) 1 + (omega) equals 2(omega) 1 - (omega) 2. In this case (omega) 3 coincides with the anti- Stokes Raman frequency associated with the molecular frequency (omega) . This process of coherent anti-Stokes Raman Scattering (CARS) is an important nonlinear optical process which provides intense collimated signal beams and is also an excellent spectroscopic tool. CARS being a four-wave mixing process, it is of interest to study the process in multi-level system to obtain a better insight into the problem. In the current paper we investigate the different quantum statistical properties of CARS in a inhomogeneously broadened three-level system based on density-matrix formalism where both the atomic system and the radiation fields are quantised. The photon-statistics, coherence characteristics and the occurrence of anti-bunching of the CARS field, in the steady state, are investigated.
Statistical properties of light produced in spontaneous Raman scattering on an ensemble of molecules indicate the quantum nature of this phenomenon. The scattered light is non-classical and has high non-classical intensity correlations between Stokes and anti-Stokes components. The temporal coherence of this light is well investigated, while many questions related to spatial coherence remain open. Recent experiments reveal two peculiar features of the spatial coherence of the Stokes and anti-Stokes light. First, the intensity correlations between Stokes and anti-Stokes light remain non-classical even for macroscopic samples containing many molecules. Second, these correlations decrease when signal propagates through a multi-mode optical fiber: the more propagating fiber modes at Stokes and anti-Stokes frequencies the less the correlations. Moreover, the second-order autocorrelation function of Stokes and anti-Stokes light also decreases with the number of propagating modes in multi-mode fiber. In this paper, we build a model of spontaneous Raman scattering correlations of light produced by an ensemble of molecules and propagating through weakly guiding optical fiber that quantitatively explains all these observations. We show that spacial orthogonality of the fiber modes makes the light propagating through these modes uncorrelated in the standard detection scheme. This leads to suppression of non-classical intensity correlations of the total field in the multi-mode fiber. We find the degree of non-classical correlations on fiber parameters. The obtained results pave the way for engineering of non-classical Stokes -- anti-Stokes correlations.
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.