The major parasitic modes of backward Raman amplifiers are different forms of superfluorescent forward Raman scattering. It is shown that spatial, and/or temporal variation of the Raman frequency in the scattering medium can inhibit amplification of spontaneously scattered light by creating off-resonant conditions in the forward direction. If the frequencies of the optical pulses are properly varied in time (the pulses are chirped), the required resonance condition for amplification of a counterpropagating Stokes wave can be maintained throughout the medium. Raman transition frequencies can be varied in an atomic vapor by application of a magnetic field via the Zeeman effect. The use of thallium (T1) metal vapors for scattering XeCl or KrF excimer laser radiation is considered as a particular example.
The major parasitic modes of backward Raman amplifiers are different forms of superfluorescent forward Raman scattering. It is shown that spatial, and/or temporal variation of the Raman frequency in the scattering medium can inhibit amplification of spontaneously scattered light by creating off-resonant conditions in the forward direction. If the frequencies of the optical pulses are properly varied in time (the pulses are chirped), the required resonance condition for amplification of a counterpropagating Stokes wave can be maintained throughout the medium. Raman transition frequencies can be varied in an atomic vapor by application of a magnetic field via the Zeeman effect. The use of thallium (T1) metal vapors for scattering XeCl or KrF excimer laser radiation is considered as a particular example.
Raman oscillation, frequency upconversion, and Raman amplification can be achieved in a second-order nonlinear medium at the phonon-polariton resonance. By beating two optical fields, a second-order nonlinear polarization is generated inside the medium. Such a polarization induces a spatially uniform nonpropagating electric field at the beat frequency, which in turn mixes with the input optical field at the lower frequency to generate or amplify the anti-Stokes optical field. Raman oscillation can be efficiently reached for the copropagating configuration. In comparison, efficient frequency upconversion and large amplifications are achievable for the counterpropagating configuration. These Raman processes can be used to effectively remove transverse-optical phonons before decaying to lower-frequency phonons, achieve laser cooling, and significantly enhance coherent anti-Stokes Raman scattering. The counterpropagating configuration offers advantages for amplifying extremely weak signals.
In the case of the scattering Raman amplification of light beams in a field of powerful ultrashort pulses, the back influence of the amplified radiation on the fundamental wave may be significant. Moreover, properties of the media, such as a population of atomic states, may significantly change. That leads to amplitude-phase modulation of the fundamental pulse owing to change of direction of intensity exchange in the pulse.1 As a result, the bond between the fundamental and Stokes waves becomes weaker, that results in a decrease in the frequency conversion efficiency. For spatial inhomogeneous beams this effect is different in various beam sections.
A pencil shaped region of a Raman-active medium forms a source for Stokes-shifted light via stimulated Raman Scattering (SRS) when driven by an intense laser pulse. Stokes photons are scattered spontaneously at first, and then amplified during propagation through the medium. Since the scattering is initiated by quantum noise, the actual number of photons produced in any given pulse will be highly uncertain, even if the pulse energy of the driving laser is constant1. As the Stokes light propagates through such an extended region, it's coherence properties will be changed. The spatial coherence is determined by the size and shape of the region, which may be characterized by its Fresnel number F, defined as F= A/λSL, where A is the cross-sectional area of the interaction region, which has length L, and λS is the Stokes wavelength. The rate at which the microscopic scatterers (atoms or molecules) are dephased by collisions affects the temporal coherence of the Stokes light, characterised by the temporal coherence parameter Γτ /gL, where Γ is the collisional dephasing rate, τ is the laser pulse duration and g is the steady-state Raman gain coefficient.
Technological progress in commercializing ultrafast lasers and detectors has allowed realization of cooperative processes on an ultrashort time scale, which demand a re-evaluation of the conventional cooperative phenomena with a new insight. Ultrafast cooperative phenomena in coherently prepared media and various applications of superfluorescence and coherent Raman scattering are studied in this dissertation. In particular, a simple theoretical testimony on analogy between a cooperative emission and coherent Raman scattering is presented by offering an opportunity to perform parallel research on these two processes from a unified point of view.\n\nOn one hand, the superfluorescent pulse with a time duration of a few tens of picoseconds (ps) from alkali metal vapor is observed for the first time, even though cooperative phenomena in atomic vapor have been extensively studied for more than five decades. A dense rubidium vapor pumped by ultrashort (100 femtosecond, fs) pulses allows a realization of the ultrafast superfluorescence while a time-resolved study of superfluorescence is accomplished by using a streak camera with 2 ps time resolution. Experimental research on quantum nature of cooperative emissions has been “frozen” over the years (three decades) possibly because of the technical difficulties. Quantum fluctuations of superfluorescence development are explored experimentally by taking advantage of the ultra fast streak camera. Presumable applications of the superfluorescent pulse in e.g., a remote sensing, and an ultraviolet upconversion of the input infrared laser pulse are presented. The quantum interference due to different excitation pathways is revealed by the temporal coherent control technique while observing interferometric signals from alkali metal vapors. \n\nOn the other hand, a new spectroscopic technique based on ultrafast coherent Raman scattering is developed. The key advantage of the presented technique is to suppress the non-resonant background noise which usually obscures possible applications of the other conventional coherent Raman techniques in practice. A reduction of the background noise is achieved by shaping and delaying the third pulse which probes the coherence of the medium (i.e., an enhancement of specific vibrations of the target molecules in unison) firstly prepared by two broadband pulses. We demonstrate a robustness and superiority of signal-to-noise ratio of the developed technique by identifying as few as 10000 bacterial spores at a single laser shot level.\n\nFinally, several comparative studies between cooperative and uncooperative processes are presented. A picosecond cooperative phenomenon in a three-photon resonant medium induced by a single as well as two-color ultrashort pulses is investigated. A time-resolved study shows that a picosecond cooperative effect is crucial in the well-established fields of resonant-enhanced multiphoton ionizations and harmonic generations. We also present a quantitative analysis for spontaneous versus broadband coherent Raman scattering on pyridine molecules. The spontaneous Raman signal is enhanced by 5 orders as a result of cooperative phenomena.
A theory of stimulated Raman scattering (SRS) is presented which treats in a unified manner the buildup of SRS from spontaneous Raman scattering and the spatial propagation which leads to gain. Maxwell-Bloch equations describe the coupling between the Stokes field operator and the collective atomic operators, which are driven by a classical laser field under low-signal-gain conditions, where the atomic ground states and laser field remain undepleted. An analytic expression is derived for the forward-propagating Stokes field operator in a one-dimensional spatial approximation when the Fresnel number of the excited medium is unity. Steady-state and transient Stokes intensities are evaluated under low-gain (spontaneous) and high-gain (stimulated) conditions. The Stokes intensity is found to be exactly independent of a laser bandwidth arising solely from phase fluctuations. The power spectrum of steady-state SRS is evaluated, giving a gain-narrowed spectral profile when the laser is narrow band, and a spectrum identical to the laser spectrum when the laser is broad band. A strong analogy between SRS and two-level superfluorescence is found; in both cases the macroscopic, collective dipole moment is initiated by quantum fluctuations.
This chapter shows that solitons and other special solutions of soliton equations play important roles in helping people understand the transverse structure of optical beams in optical cavities, the longitudinal structure of pulses in resonant media, superfluorescence, and the production of the Stokes wave in Raman scattering processes. It describes the fundamental ingredients required for laser operation. The chapter introduces the simplest model of a laser involving a medium of two-level atoms. It discusses the manifestation of optical bistability in ring and Fabry–Perot cavities. The chapter also discusses the stability of the "stable" solutions and find that they can undergo a series of period-doubling bifurcations leading to a temporally chaotic output. It looks at the remarkable behavior of a pulse propagating through an almost perfectly tuned resonant and initially passive medium. The resonator is tuned to support frequencies close to that of the laser transition.