Superradiance and Raman scattering in three-level molecular system

A model is presented for the dynamics of superradiance, coherent and stimulated Raman scattering from an optically pumped three-level system. The evolution of the pumping and two counterpropagating waves in the adjacent transition are taken into account. The results of computer simulation show that by specifying the pumping pulse area, and active medium length and pressure we can control the parameters of the pulses in the adjacent transition. The possibilities of observing coherent Raman scattering dynamics, which are significantly different from that for stimulated Raman scattering, are shown. The results of simulation show that for the ultrashort pumping pulse the superradiative emission in the backward direction is formed within the coherence length near the entrance plane of the active medium.     

Creation of arbitrary coherent superposition states in four-level systems

Using the technique of stimulated Raman adiabatic passage, we propose schemes for creating arbitrary coherent superposition states of atoms in four-level systems: a Λ-type system with twofold final states and a four-level ladder system. With the use of a control field, arbitrary coherent superposition states are created without the condition of multiphoton resonance. Suitable manipulation of detunings and the control field can create either a single state or any superposition states desired.     

一种用弱信号光调制的宽带光纤拉曼相干光源

本文考察了光纤中外加可调谐信号光条件下的受激拉曼散射现象,提出一种新的宽带光纤拉曼相干光源的设想。这种光源是利用波长可调的弱信号光来调制固定波长的强泵浦光在光纤中产生的高阶受激拉曼散射,使得高阶受激拉曼散射Stokes峰值波长随弱信号光的波长改变而改变。从而获得一个输出均匀而频带又比信号光宽得多的高强度相干光。     

Applications of stimulated Raman scattering

The applications of stimulated Raman scattering reviewed in this paper include: determination of spontaneous Raman parameters and nonlinear susceptibilities by gain measurements and coherent anti-Stokes Raman spectroscopy, excitation of molecular vibrations and lattice waves and measurement of their relaxation times, generation of intense tunable light in the infrared region of the spectrum. The main results of the theory of stimulated Raman scattering relevant to the understanding of these applications are discussed.     

Experimental demonstration of selective coherent population transfer via a continuum

We report the first experimental demonstration of coherent population transfer, induced by stimulated Raman adiabatic passage, via continuum states. Population is transferred from the metastable state 2s(1)S(0) to the excited state 4s(1)S(0) in helium atoms in a two-photon process mediated by coherent interaction with the ionization continuum. While incoherent techniques usually do not permit any population transfer in such a process, we show that stimulated Raman adiabatic passage allows significant population transfer to take place also via ultrafast decay channels.     

利用受激Raman跃迁制备的原子激光的相干性

研究了利用原子玻色-爱因斯坦凝聚体与制备的原子激光的二阶相干性质. 结果表明,这种原子激光是反聚束的,在一定条件下,是二阶相干的.     

Experimental observation of different-order components of a vibrational wave packet in a bulk dielectric using high-order Raman scattering

We use high-order Raman scattering in a bulk dielectric to characterize coherent dynamics with precision typical for gas phase experiments. The experimental pump-probe approach allows for the simultaneous observation and separation in space and time of the individual contributions of different-order Raman processes to a coherent wave packet without relying on phase-matching conditions and within the same experimental geometry. We propose a novel technique to discriminate between stimulated excitation of vibronic levels in the impulsive and intermediate excitation regimes, futhermore allowing us to distinguish between different pathways contributing to the same fifth-order Raman processes.     

利用受激Raman跃迁制备的原子激光的相干性

研究了利用原子玻色-爱因斯坦凝聚体与光相互作用产生受激Raman跃迁制备的原子激光二阶相干性质。结果表明,这种原子激光是反聚束的,在一定条件下,是二阶相干的。     

双Λ型原子系统中制备相干叠加态的研究(英文)

本文讨论了在双Λ型原子系统中制备相干叠加态的方法:一个Λ型系统通过控制激光而另一个Λ型系统采用部分受激拉曼绝热通道的方法.在理论上分析了产生任意相干叠加态的可能性并且讨论了透热系统在产生相干叠加态过程中的重要性.研究表明,没有透热过程是不可能制备出任意的叠加态.应用数值方法验证理论分析是正确,并且指出任意叠加态的产生只与控制脉冲的时间延迟有关.     

驱动激光束间相干性以及对背向散射影响的研究

早期的研究表明, 束匀滑技术能够有效地抑制高功率激光与等离子体相互作用中产生的各种参量不稳定性, 大大减少受激布里渊散射和受激拉曼散射. 但在NIF最近的实验研究中发现, 受激布里渊散射和受激拉曼散射份额远远高于预期, 原因可能与驱动激光束间的相干性有关. 本文利用"神光II"装置两路倍频纳秒激光辐照金平面靶, 研究了小口径取样情况下两者背向散射的能量和光谱在不同驱动激光相干条件下的变化情况. 初步结果表明, 激光束间存在着较强的相干性, 并且随着束间相干程度的增加, 背向散射也逐渐增强.     

Ultrafast control of coherent population transfer with a train of femtosecond pulse pairs

We investigate the ultrafast control of coherent population transfer in a Λ-type three-level system with a train of pump-Stokes femtosecond pulse pairs, where the pulse sequences can be produced either by optical delay line or by pulse shaping with sinusoidal phase modulation. It is shown that when the pump and Stokes pulses in each pair are applied in the counterintuitive order, similar to that in the stimulated Raman adiabatic passage technique, due to temporal quantum interference (besides optical interference in the case of overlapped subpulses), ultrafast control of coherent population transfer can be achieved by scanning the inter-pair time delay or by changing the sinusoidal phase modulation parameters. This method has potential applications in ultrafast control of chemical reactions and quantum information processing.     

Laser-induced gratings in the gas phase excited by Raman-active transitions

We report on a new time-resolved coherent Raman technique that is based on the generation of thermal gratings following a population change among molecular levels that is induced by stimulated Raman pumping. This is achieved by use of spatially and temporally overlapping intensity interference patterns generated independently by two lasers. When this technique is used in carbon dioxide, making use of transitions that belong to the Q branches of the v(1)/2v Fermi dyad, it is possible to investigate molecular energy transfer processes. A further unique feature of this method is spectral resolution that is better than that achieved by coherent anti-Stokes Raman scattering.     

Generation of three-primary-color Raman comb in the continuous-wave regime

We demonstrate the generation of continuous-wave Stokes and anti-Stokes Raman sidebands including the three-primary-color (683, 532, and 436 nm) components. The Raman sidebands are generated through both stimulated and coherent anti-Stokes Raman scattering in a broadband high-finesse optical cavity filled with gas-phase hydrogen as a Raman-active medium and covering the entire visible spectral range (420–680 nm). The blue emission is considerably enhanced by matching the frequency with one of the longitudinal modes of the optical cavity, and high conversion efficiencies are observed when the coherent length corresponds to an integral multiple of the round-trip length of the optical cavity. This indicates that phase-matching plays a critical role in determining the efficiency of the Raman comb generation.     

Superposition of Fock states via adiabatic passage in a coupled four-level atom－cavity system

We have investigated the behaviour of an atom－cavity system via a stimulated Raman adiabatic passage technique in a four-level system, in which two dark states are present. We find, because of the coherent control field, that a superposition of Fock states can be prepared, even when the cavity is initially not in its vacuum state. This method provides a way to generate arbitrary quantum states of a cavity field.     

White-light parametric instabilities in plasmas

Parametric instabilities driven by partially coherent radiation in plasmas are described by a generalized statistical Wigner-Moyal set of equations, formally equivalent to the full wave equation, coupled to the plasma fluid equations. A generalized dispersion relation for stimulated Raman scattering driven by a partially coherent pump field is derived, revealing a growth rate dependence, with the coherence width sigma of the radiation field, scaling with 1/sigma for backscattering (three-wave process), and with 1/sigma1/2 for direct forward scattering (four-wave process). Our results demonstrate the possibility to control the growth rates of these instabilities by properly using broadband pump radiation fields.     

Characterization of a supercontinuum generated from a photonic crystal fiber and its application to coherent Raman spectroscopy

The temporal and spectral profiles of supercontinuum radiation generated from a photonic crystal fiber are evaluated with a polarization-gate frequency-resolved optical gating technique. The supercontinuum is then applied to coherent inverse Raman spectroscopy. A stimulated Raman signal of cyclohexane is observed as an induced absorption signal with an instantaneous response. The Raman signal has a peak at a slight negative delay time, which is explained by perturbed Raman-induced coherence.     

Induction of the maximum Raman coherence in an extended medium through fractional adiabatic passage

The effect of fractional stimulated Raman adiabatic passage in an optically dense medium of three-level Λ atoms is shown to result in the maximum coherence on the Raman transition on a length of the medium that considerably exceeds the length of linear resonant absorption. The general case of unequal oscillator strengths of the adjacent transitions is analyzed. The results are of interest for coherent anti-Stokes Raman spectroscopy with delayed pulses.     

Stimulated and spontaneous optical generation of electron spin coherence in charged GaAs quantum dots

We report on the coherent optical excitation of electron spin polarization in the ground state of charged GaAs quantum dots via an intermediate charged exciton (trion) state. Coherent optical fields are used for the creation and detection of the Raman spin coherence between the spin ground states of the charged quantum dot. The measured spin decoherence time, which is likely limited by the nature of the spin ensemble, approaches 10 ns at zero field. We also show that the Raman spin coherence in the quantum beats is caused not only by the usual stimulated Raman interaction but also by simultaneous spontaneous radiative decay of either excited trion state to a coherent combination of the two spin states.     

Femtosecond stimulated Raman scattering picosecond molecular thermometry in condensed phases

We demonstrate the capability of femtosecond stimulated Raman scattering (FSRS) data to measure the temperature of condensed matter at the molecular vibrational level. We report the temperature dependence of Raman loss to Raman gain ratios for low frequency modes (<300 cm(-1)) in a CaCO3 single crystal from cryogenic to room temperature, which is shown to be in agreement with theoretical predictions. We also report the measurements of nonequilibrium time evolution of mode specific vibrational temperatures in the CaCO3 single crystal to demonstrate that FSRS can measure temperature on picosecond time scales. Finally, we point out the unique origin of this temperature dependent anti-Stokes to Stokes ratio in stimulated Raman, which is not present in other coherent Raman spectroscopies. These measurements require no material dependent parameters or prior calibration.