Generation of a dark nonlinear focus by spatio-temporal coherent control

The transition probability of a two-photon absorption (TPA) process in atomic Cesium, excited by phase-controlled temporally focused ultrashort pulses is shown to be spatially modulated in a controlled manner. In particular, we demonstrate the generation of a dark nonlinear focus. By controlling the excitation pulse shape along the propagation coordinate we create a region in space where the TPA rate vanishes which is flanked by bright regions.     

Coherent enhancement of broadband frequency up-conversion in BBO crystal by shaping femtosecond laser pulses

An optimal feedback control of broadband frequency up-conversion in BBO crystal is experimentally demonstrated by shaping femtosecond laser pulses based on genetic algorithm, and the frequency up-conversion efficiency can be enhanced by ∼16%. SPIDER results show that the optimal laser pulses have shorter pulse-width with the little negative chirp than the original pulse with the little positive chirp. By modulating the fundamental spectral phase with periodic square distribution on SLM-256, the frequency up-conversion can be effectively controlled by the factor of about 17%. The experimental results indicate that the broadband frequency up-conversion efficiency is related to both of second harmonic generation (SHG) and sum frequency generation (SFG), where the former depends on the fundamental pulse intensity, and the latter depends on not only the fundamental pulse intensity but also the fundamental pulse spectral phase.     

Controlled generation of single photons from a strongly coupled atom-cavity system

We propose a new method for the generation of single photons. Our scheme will lead to the emission of one photon into a single mode of the radiation field in response to a trigger event. This photon is emitted from an atom strongly coupled to a high-finesse optical cavity, and the trigger is a classical light pulse. The device combines cavity-QED with an adiabatic transfer technique. We simulate this process numerically and show that it is possible to control the temporal behaviour of the photon emission probability by the shape and the detuning of the trigger pulse. An extension of the scheme with a reloading mechanism will allow one to emit a bit-stream of photons at a given rate. Received: 7 July 1999 / Revised version: 3 September 1999 / Published online: 20 October 1999     

Observation of Sub-femtosecond Polarization Beats Using Twin Noisy Driving Fields

We study the phase-conjugate polarization interference in a V-type three-level system and obtain an analytic closed form for the second-order stochastic correlation of sum-frequency polarization beat. In our Na vapour atomic system pumped by laser pulse of nano-second timescale duration, we experimentally demonstrate an ultrafast modulation of the four-wave mixing signal intensity with a sub-femtosecond timescale period, corre- sponding to the sum-frequency of the resonant transitions from 3S1/2 to 3Pl/2 and 3P3/2.     

Dressed Four-Wave Mixing Spectroscopy Modified by Polarization Interference and Atom-Wall Collision in Micrometric Thin Cells

Dressed four-wave mixing （DFWM） spectroscopy is investigated theoretically in some micrometric thin cells. It is found that DFWM spectra can be modified by polarization interference of atoms and transient effects induced by atom-wall collision. This modification can lead to width-narrowing of DFWM lines and facilitates to implement experiment of high resolution DFWM spectroscopy in a confined atomic system.     

Sub-Half-Wavelength Atom Localization via Coherent Control of Autler-Townes Spontaneous Spectrum

We show that it is possible to localize an atom in a half-wavelength region by relaxing the strict condition that the atom is prepared in a specific excited state as in the recently proposed scheme [Phys. Rev. A 65 （2002） 043819]. In particular, we consider a four-level atom, for which a weak exciting field transfers population from the ground state to the excited state and three control fields （one standing-wave field while two travelling-wave fields） couple the excited state and two auxiliary states. By tuning the exciting field and by varying the collective phase of the control fields, the atom is localized in one of the two half-wavelength regions with 50% detecting probability. The main advantage of the scheme is the experimental accessibility and controllability.     

Interactions of Three Dual-Dressing Effects of Four-Wave Mixing in a Five-Level Atomic System

We study the four-wave mixing （FWM） in an opening five-level system with two dressing fields. There axe three kinds of doubly dressing mechanisms （parallel cascade, sequential cascade, and nested cascade） in the system for doubly dressed four-wave mixing. These mechanisms reflect different correlations between two dressing fields and different effects of two dressing fields to the FWM. Investigation of these mechanisms is helpful to understand the generated high-order nonlinear optical signal dressed by multi-fields.     

Interaction of Triply-Dressing Electromagnetically Induced Transparency in Five-level Folding Atomic System

We consider a five-level atomic folding system, which involve two kinds of dressing mechanisms （the nested- cascade and the sequential-cascade） in interaction of three-dressing fields, the numerical results show that three- dressing fields are interchangeable under certain conditions, which can be considered as two four-level sub-system configurations （a nested-cascade N configuration and a sequential-cascade inverted-Y configuration）.     

Coherent Phase Control of Ultrafast Polarization Beats in Reverse V-Type Three-Level System

We investigate the third-order nonlinear absorption and dispersion of femto- and atto-second polarization beats between the one-photon degenerate four-wave mixing process and the two-photon nondegenerate four-wave mixing process in the pure homogeneously-broadened reverse V-three-level using twin noisy fields. The third-order nonlinear response can be controlled and modified by the colour-locked correlation of twin noisy fields. Most importantly, the coherent phase control in optical heterodyne detection for studying the phase dispersion of the third-order susceptibility is demonstrated. The radiation-matter detuning oscillation is also considered in the freauencv domain.     

Competition between Dispersion and Absorption of Doubly-Dressed Four-Wave Mixing and Dressed Six-Wave Mixing

We study the competition between dispersion and absorption of doubly-dressed four-wave mixing （DDFWM） and dressed six-wave mixing. In the case of weak coupling fields limit, we find DDFWM signal is affected by destructive interference between four-wave mixing（FWM） and six-wave mixing as wen as constructive interference between FWM and eight-wave mixing. By analysing the difference between two kinds of doubly dressing mechanisms （parallel cascade and nested cascade） in this opening five-level system, we can further understand the generated high-order nonlinear optical signal dressed by multi-fields.     

Dicke-Narrowing Spectroscopy of Doubly Dressed Electromagnetically Induced Transparency and Singly Dressed Four-Wave-Mixing in a Confined Atomic System

Dicke-narrowing effect appears both in doubly dressed electromagnetically induced transparency and singly dressed four-wave-mixing lines due to the contribution of slow atoms resulting from de-excited effects of atom-wall collision and transient behaviour of atoms in a confined system. A robust recipe for high resolution spectroscopy of electromagnetically induced transparency dressed by two fields and four-wave-mixing lines comparable with the cold atoms is achievable in a thin vapour cell in experiments.     

Trichromatic Manipulation of Kerr Nonlinearity in a Three-Level Λ Atomic System

Trichromatic manipulation of Kerr nonlinearity in a three-level ∧ atomic configuration is investigated theoretically. It is Shown that for a weak monochromatic probe field, the enhanced Kerr nonlinearity can be achieved in multiple separate transparent windows due to interference effect of multiple two-photon Raman channels. Furthermore, the property of Kerr nonlinearity can be controlled by the sum of the relative phases of the sideband components of the trichromatic pump field compared to the central component.     

Enhancement of Bichromatic High-Order Harmonic Generation by a Strong Laser Field and Its Third Harmonic

We investigate high-order harmonic generation （HHG） in a linearly polarized bichromatic field composed of a fundamental laser field with frequency w and an additional laser field with frequency 3w. The numerical results show that it is possible to enhance the intensity of most high harmonics in orders of magnitude. A most striking feature in the enhancement is that the intensity of several special high harmonics is practically impaired as compared with that in the monochromatic case. The qualitative explanation to the great enhancement is that the additional high-frequency field can provide new transition paths for electrons to reach the continuum. The relative phase between the fundamental field and its third harmonic field also affects the intensity of high-order harmonics near the cutoff efficiently.     

Optimal control of one- and two-photon transitions with shaped femtosecond pulses and feedback

This paper reports two pump–probe experiments in sodium where dynamically tailored ultrashort pulses from a Ti:Sapphire-pumped optical parametric amplifier were employed. The first study focuses on the one-photon Na(3s→3p) transition to derive sensitive criteria which judge the performance of a frequency-domain pulse shaper using a spatial light modulator. On the basis of the interpretation, follow-up experiments are suggested to test their cogency. The second experiment uses coherent quantum control by placing an appropriate phase distribution on the incident beam to enhance or cancel the transition probability in the nonresonant two-photon process Na(3s→→5s). Ignorant of the “ideal” phase function, an evolutionary algorithm which uses a feedback derived from the experiment performs the optimization and produces the desired bright or dark pulses within a few minutes. Attention is given to the role of resonant 3s→3p transitions excited by the spectral wings of the pump pulse. Different parametrizations of the phase distribution have been examined. Two of these produced solutions which had not previously been predicted by theory still meet the objective of the experiment. The study represents the first successful application of a feedback-organized self-learning algorithm to the design of dark pulses. Received: 3 November 1999 / Published online: 5 July 2000     

The impact of laser field statistics in determination of temperature and concentration by multiplex USED CARS

Experiments have been performed which demonstrate that the ratio of resonant to nonresonant third-order susceptibilities measured in multiplex USED CARS are affected by the time correlation of the pump fields. Comparing the resonant to nonresonant signal ratio obtained with decorrelated fields to the ratio obtained with correlated fields, a relative increase of 2.5 was measured for the nitrogen Q-branch, whereas a corresponding increase of 1.9 was observed for the hydrogen Q(1)-line. To compare our experimental results with theoretical calculations of the spectral shapes, the nonresonant third-order susceptibilities of a number of gases were re-evaluated by calibrating to the nonresonant susceptibility of argon.     

Is rotational CARS an alternative to vibrational CARS for thermometry?

Recent developments in rotational CARS thermometry and critical issues when comparing vibrational and rotational CARS thermometry are described. In particular, the development of dual broadband rotational CARS and the noise characteristics of this approach are emphasized. The difficulty with unambiguous temperature determination in vibrational CARS with unknown parameters, in particular the nonresonant background susceptibility, and the lower sensitivity of rotational CARS thermometry at flame temperatures are also discussed.     

Ultrabroadband single-pulse CARS of liquids using a spatially dispersive Stokes beam

A double-channel spectrometer, which enables to acquire ultrabroadband single-pulse spectra of liquids by Coherent Anti-Stokes Raman Spectroscopy (CARS), is described. The method used to fulfill the phase-matching condition is based on the fact that the CARS efficiency in dispersive media is the largest when the interactive waves cross each other under frequency-determined angles. The dependence of the spatial separation between the pump and Stokes beam, in front of the crossing CARS lens, due to their frequency difference is analysed. It is shown that the different spectral components of an ultrabroadband Stokes source have phase-matched the CARS process when they are laterally shifted by a conjugated prism pair and focused into the sample. The method is tested in the spectral region 2800–3800 cm^–1 of a non-resonant medium (CCl₄) using an ultrabroadband dye laser (1000 cm^–1 FWHM). The influence of the Stokes beam spatial dispersion on the width of CARS generation is demonstrated. By this method, 1060 cm^–1 wide single-pulse spectra of the OH stretching vibration of liquid water are obtained for the first time. The ratio between the resonant and non-resonant part of the third-order susceptibility in water and methanol is determined.     

Generation of Continuum Extreme-Ultraviolet Radiation by Carrier-Envelope-Phase-Stabilized 5-fs Laser Pulses

Coherent extreme-ultraviolet （XUV） radiation is studied by interaction of carrier-envelope （CE） phase stabilized high energy 5-fs infrared （800 nm） laser pulses with neon gas at a repetition rate of 1 kHz. A broadband continuum XUV spectrum in the cut-off region is demonstrated when the CE phase is shifted to about zero, rather than modulated spectral harmonics when setting of CE phase is nonzero. The results show the generation of isolated attosecond XUV pulses.     

CARS thermometry in high temperature gradients

CARS is an effective non-intrusive technique for measuring gas temperature in combustion environments. In regions of high temperature gradient, however, the CARS signal is complicated by contributions from gas at different temperature. This paper examines theoretically the uncertainty associated with CARS thermometry in steep temperature gradients. In addition, the work compares the temperature predicted from CARS with the adiabatic mixed temperature of the gas resident in the measurement volume. This comparison helps indicate the maximum sample volume size allowed for accurate temperature measurements.     

High-Order Above-Threshold Ionization of H2+ in Intense Laser Field

The nonperturbative quantum electrodynamies method proposed by Fu et al. [Phys. Rev. A 75 （2007） 063419] is employed to study the high-order above-threshold ionization （ATI） of a diatomic molecule. Based on this frequency-domain theory, the high-order ATI process can be regarded as ATI followed by laser-assisted collision, where the total transition amplitude is the coherent summation of the contributions from each ATI channel. The angular-resolved ATI spectrum, which agrees with the results by Becket et al. based on the time-domain method, is obtained by this frequency domain theory. Furthermore, it is demonstrated that the interference characteristics representing the molecular structure in the ATI spectrum originates from the recollision of the electron with two-centre ion in each ATI channel.