Gas-phase velocimetry by nearly degenerate four-wave mixing

We demonstrate a new velocimetry technique for gas flows based on Nearly Degenerate Four-Wave Mixing (NDFWM). Measurements were performed on nitric oxide in a free-jet expansion using helium and argon as carrier gases, at flow velocities on the order of 1000 m/s. We obtained velocities by analyzing experimental spectra from the jet using a perturbative treatment of NDFWM that we extended to include an arbitrary bulk velocity. The results agreed with independent velocity measurements based on Laser-Induced Fluorescence (LIF), as well as with theoretical flow-field velocities, to better than 5% in all cases studied.     

The pressure effect on the photoluminescence and Raman spectra of Nd(DBM)3·Phen

Photoluminescence and Raman spectra of rare earth complex Nd(DBM)₃·Phen (DBM, dibenzoylmethane; Phen, 1,10-phenanthroline) are measured at high pressures. A new Raman band appearing at 1070 cm⁻¹ indicates a second-order phase transition around 5.0 GPa. Although the crystal lattice is destroyed for pressures higher than 7.1 GPa, photoluminescence spectra show that the emission intensity of Nd³⁺ is enhanced dramatically with the pressure increasing up to 9.9 GPa, which is attributed to an efficient intramolecular energy transfer from the ligand to Nd³⁺. By analyzing the energy of the ground and excited states at 9.9 GPa, the ⁴H_11/2 energy level is considered as the main resonance energy level that efficiently accepts the transferred energy from the ligand.     

Picosecond phase-conjugation by degenerate four-wave mixing in sodium vapour

Phase-conjugated waves (PCW), via degenerate four-wave mixing (DFWM) with picosecond laser pulses having a FWHM of 80 ps have been obtained in sodium vapour on both sides of theD ₂(3² S _1/23² P _3/2) transition at 589 nm. The maximum reflectivity of the PCW signals was 60%. The reflectivity of the PCW has been measured as a function of the temperature, the detuning and the pump and probe intensities. Because of the very strong nonlinear behaviour of theD ₂ transition the appearance of the PCW is accompanied by strong self-focusing and defocusing of the beams, which give a rather complicated line-shape of the detuning curve of the PCW. By varying the delay between the beams, the lifetime of the transient volume grating has been, measured to be 7.4 ns. The results are in qualitative agreement with the theoretical model of Abrams and Lind.     

Luminescence and Energy Transfer of Eu^2＋, Mn^2＋ in SrZnP2O7

The SrZnP2OT：Eu^2＋, Mn^2＋ phosphor is synthesized by high temperature solid state reaction. The luminescence properties and the energy transfer between Eu^2＋ and Mn^2＋ are investigated. The emission bands of this phosphor peaked at 42Ohm and 67Ohm are originated from the 5d → 4f transition of Eu^2＋ and from the 4T1 （4G） --〉 6A1 （6S） transit/on of Mn^2＋, respectively. With the increasing Mn^2＋ concentration, the intensity of fixed concentra- tion Eu^2＋ decreases and the intensity of Mn^2＋ also increases. It is suggested that there is an energy transfer from Eu^2＋ to Mn^2＋ in SrZnP2O7 host. According to Dexter＇s energy transfer formula of multipolar interaction, the energy transfer between Eu^2＋ and Mn^2＋ is due to the electric dipole-quadrupole interaction of the resonance transfer.     

Highly efficient inelastic four-wave mixing using dual induced transparency and coherently prepared states

We investigate a life time broadened and coherently prepared five-state system for multi-wave mixing processes. We show that very efficient wave mixing occurs, producing an unconventional mixing wave that has the characteristics of both conventional four-wave mixing (FWM) and stimulated hyper-Raman (SHR) emission. In addition, we show interesting multiple simultaneous multi-photon interference effects at large propagation distances and demonstrate more than 10 orders of magnitude suppression of populations of the probe wave terminal state and the near three-photon resonance mixing wave generating state. These new type of multi-photon interference based induced transparency effects, which are critically dependent on two distinctive relaxation processes involving both an external supplied and an internally generated fields, are fundamentally different from the conventional three-state electromagnetically induced transparency effect which does not depend on propagation. As a consequence, both the probe and the wave-mixing field to propagate nearly free of absorption and distortions in a highly dispersive medium.     

Stability of localized structures in degenerate wave mixing

We give experimental proof of the stability of (supercritical) spatial phase solitons in degenerate wave mixing. Received: 16 June 1999 / Published online: 25 August 1999     

Femtosecond Kerr ellipsometry in polydiacetylene solutions: Two-photon effects

We describe a pump-probe femtosecond Kerr experiment in polydiacetylene solutions (4BCMU, yellow form). The Kerr ellipsometry technique permits a separate determination of the real and of the imaginary part of anisotropic index changes. The wavelength (620 nm) of the pump pulses lies in the transparency region of polydiacetylene while the probe pulses have a broad white spectrum. The largest contribution to the Kerr signal is a quasi-resonant stimulated anti-Stokes Raman absorption. A flat two-photon transition spectrum with 4×10^–3 cm/MW is observed close to 4 eV. The two-photon excited states have a life time close to 12 ps and they present a broad absorption band in the 2 eV range.     

Synthesis of and excited state processes in multichromophoric dendritic systems

Rigid polyphenylene dendrimers substituted with dyes are suitable substrates for the investigation of interchromophore photophysical processes as they contain discrete numbers of chromophores in well-defined spatial relationships to each other. In this contribution, we provide an overview of the synthesis of such materials and show how a combination of ensemble and single-molecule spectroscopic investigations can be used to elucidate the interchromophore excitation energy transfer processes in them.     

Experimental investigation of the effect of collisions and temperature on degenerate four-wave mixing

An experimental investigation (including a comparison with a simple theoretical model) of the effect of buffer-gas composition, pressure and temperature on resonant Degenerate Four-Wave Mixing (DFWM) has been performed. The DFWM signal from NO in a quartz cell was measured and the effect of quenching as well as elastic (phase-changing) collisions was studied by varying the total and partial pressures of N₂ and CO₂ as buffer gases. It was found that the DFWM signal first slowly increased with buffer-gas pressure (up to 10 mbar) and then rapidly decreased. It was furthermore found that the DFWM signal was considerably less sensitive to quenching collisions as compared to Laser-Induced Fluorescence (LIF) (for laser intensities approximately equal to half the DFWM saturation intensity of the transition). On the other hand, while LIF is virtually insensitive to elastic collisions, DFWM displays a larger sensitivity to elastic collisions than to quenching collisions. The DFWM saturation intensity was found to increase with buffer-gas pressure (although slower than expected). When varying the temperature of the gas composition, it was found that the DFWM signal decreased markedly with increasing temperature. This decrease is too fast to be explained solely by a change in the population of the molecular state probed by the laser.     

Characterization of ultra-weak fluorescence using picosecond non-collinear optical parametric amplifier

We report a technique for characterization of ultra-weak fluorescence based on a 355-nm pumped picosecond non-collinear optical parametric amplifier (OPA). In the experiment, we effectively reduced the strong super-fluorescence background by using a series of methods. With the picosecond OPA as the pre-amplifier and the gating pulse, the decay of the fluorescence of Rhodamine 6G dye in ethanol was measured and the fluorescence lifetime was found to be about 941 ps. The gain factor of this parametric fluorescence amplifier was measured to be ∼4.2 × 10⁶, while the energy detection limit was ∼160 aJ per pulse within a 15-ps gating pulse.     

Study of optical nonlinearity of functionalized multi-wall carbon nanotubes by using degenerate four wave mixing and Z-scan techniques

The phase conjugation geometry of degenerate four wave mixing (DFWM) technique has been employed to study the third-order optical nonlinear susceptibility (χ³) and second-order hyperpolarizability of multi-wall carbon nanotubes (MWCNTs). MWCNTs were grown by thermal chemical vapor deposition method and, subsequently functionalized with carboxylic acid group to improve their solubility in an organic solvent, ethylene glycol. The average hyperpolarizability for each carbon atom has been found to be 4.74 × 10⁻⁴⁶ m⁵/V² for the pump pulse of 8 ns at 532 nm. Decreasing the pulse width of the pump laser decreases the average value of hyperpolarizability. The absorption spectra show a monotonous increase from IR through visible and give an opportunity to estimate the imaginary part of the χ³ by the open aperture Z-scan technique.     

Two-Step degenerate four-wave mixing as a means to decrease pre- and post-filtering effects in optically thick media

The use of crossed beam 2-Step Degenerate Four-Wave Mixing (2S-DFWM) for decreasing pre- and post-filtering effects under optically thick conditions has been investigated. 2S-DFWM is a technique in which the DFWM process is performed between two excited states of which the lower one is populated by an ordinary laser excitation from a low lying, highly populated state. Experiments were performed on Au in an acetylene/air flame. We have shown that under conditions where ordinary (one-step) DFWM experiments are significantly affected by pre- and post-filtering effects (i.e., partly absorption of the pump, probe or signal beams prior to or after the interaction region) the 2S-DFWM technique can give virtually interference free signals. A variety of different laser beam and flame configurations have been investigated. It was found that the use of a crossed beam geometry, where the first step exciting laser is incident upon the interaction region perpendicular to the DFWM beams, completely eliminated severe pre- and post-filtering effects occurring for an ordinary single-step DFWM scheme in an optically thick medium.     

Detection of NO in a spark-ignition research engine using degenerate four-wave mixing

We report the first application of degenerate four-wave mixing (DFWM) to combustion diagnostics in a methane-fuelled internal combustion research engine. Combustion-generated NO in the spark-ignited engine was detected using scanning narrowband DFWM in a modified forward folded BOXCARS geometry. The resulting spectra of the X²Π-A²Σ⁺(0,0) band at 226 nm display an excellent signal-to-noise ratio. Extension of the technique to different engine operating conditions and to time-resolved multiplex DFWM is discussed. Received: 3 May 2001 / Revised version: 1 October 2001 / Published online: 29 November 2001     

Nonlinear optical studies of surfaces

A brief overview on second-harmonic generation and sum-frequency generation as surface analytical tools is given with a discussion on the intrinsic limitations of the techniques often encountered in the applications. The possibly of using nonlinear optical processes for surface studies has attracted increasing attention in recent years. Optical Second-Harmonic Generation (SHG) and Sum-Frequency Generation (SFG), in particular, have been well accepted as viable surface probes [1]. They have many advantages over the conventional techniques. By nature, they are highly surface-specific and has a submonolayer sensitivity. As coherent optical processes, they are capable of in-situ probing of surface in hostile environment as well as applicable to all interfaces accessible by light. With ultrafast pump-laser pulses, they can be employed to study surface-dynamic processes with a subpicosecond time resolution. These advantages have opened the door to many exciting research opportunities in surface science and technology. This paper gives a brief overview of this fast-growing new area of research.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

Intensity-induced nonlinear effects in UV window materials

Intensity-induced nonlinear effects in optical window materials have been investigated at 308 nm. The absolute two-photon absorption coefficients for fused silica, CaF₂, BaF₂, Al₂O₃ and ADP crystals have been measured by using a single 120 ps, transform-limited pulse from the second harmonic of a distributed feedback (DFB) dye laser. The nonlinear refractive index coefficient has been obtained from measurements of far-field intensity distributions.     

Two-photon degenerate four-wave mixing (DFWM) for the detection of ammonia: Applications to flames

Two-photon Degenerate four-wave mixing (DFWM) has been used for the detection of ammonia in a cell and in an atmospheric pressure flame. The NH₃ molecules were excited from the ground state X to either the C' or the B state and the DFWM signal was recorded simultaneously with the laser-induced fluorescence signal, originating from the C-A and B-A transitions, respectively. During the flame experiments sequential measurements of NH₃ and OH in an NH₃/O₂ flame were also performed.     

A study of blast waveforms detected simultaneously by a microphone and a laser probe during laser ablation

We examine blast waves generated in air during irradiation of absorbing samples with Nd: YAG laser pulses of fluences exceeding the ablation threshold. Blast waves were detected simultaneously by a wideband microphone and a laser beam deflection probe. By a comparative analysis of both signals in the time and frequency domain we investigate characteristic features of their nonlinear waveform evolution. To explain the observed phenomena we employ the weak shock solution of the point explosion model.     

Thermometry of an oxy-acetylene flame using multiplex degenerate four-wave mixing of C2

Thermometry of an oxy-acetylene flame using multiplex Degenerate Four-Wave Mixing (DFWM) of C₂ is demonstrated. More than 100 rotational transitions in thed ³ _g a ³ _u (0,0) Swan band of C₂ could be recorded simultaneously by use of a pulsed, broad bandwidth modeless laser. Temperatures were inferred by fitting temperature-dependent synthetic spectra of single- or multiple-shot averaged spectra. The strength and reliability of recorded signals together with the large number of rotational lines observed suggest that multiplex DFWM is a promising technique for minor species detection and for temporally resolved temperature measurements in luminous environments. Factors influencing the accuracy and precision of single-shot thermometry using the technique are discussed.     

High-resolution nonlinear laser spectroscopy of exciton relaxation in GaAs quantum wells

This paper describes measurements of exciton relaxation in GaAs/AlGaAs quantum well structures based on high resolution nonlinear laser spectroscopy. The nonlinear optical measurements show that low energy excitons can be localized by monolayer disorder of the quantum well interface. We show that these excitons migrate between localization sites by phonon assisted migration, leading to spectral diffusion of the excitons. The frequency domain measurements give a direct measure of the quasi-equilibrium exciton spectral redistribution due to exciton energy relaxation, and the temperature dependence of the measured migration rates confirms recent theoretical predictions. The observed line shapes are interpreted based on solutions we obtain to modified Bloch equations which include the effects of spectral diffusion.     

Biexcitonic effects in the time integrated four-wave mixing with picosecond pulses

We propose a simple method to estimate the biexcitonic contribution to the excitonic non-linearity. The method is based on the time integrated four-wave mixing (TI FWM) with picosecond pulses. The TI FWM signal, which is measured as a function of the delay between pump and test pulses, shows shift towards positive and negative time delay when the laser is tuned at the exciton and biexciton resonance, respectively. We show theoretically that the magnitude of the shift allows us to estimate the biexcitonic contribution to the third-order non-linearity at the fundamental band edge.