Sound-velocity measurements in gases by laser-induced electrostrictive gratings

Laser-induced electrostrictive gratings have been applied to measure the adiabatic sound velocity in various gases on a single-pulse basis. The gratings are generated by the interference of two parallel polarized, crossed excitation beams arising from a pulsed Nd: YAG laser at 532.1 nm, and are detected by diffracting a probe beam originating from a cw Ar⁺ laser operating single-line at 514.5 nm. Measurements were performed in the overlap volume of unfocused and focused excitation beams. Using unfocused beams, the sound velocities in various gases at pressures of 5 bar were measured with a statistical error for single-pulse measurements of about 0.3%. With focused beams, the accuracy of the measurements is reduced because of the propagation of the sound waves out of the smaller overlap volume of 0.2 mm diameter and 4 mm length. Measurements with focused beams were performed in air and CO₂, with an error of about 1%.     

Gas-phase diagnostics by laser-induced gratings II. Experiments

In this article we review the results achieved in the past ten years at the Paul Scherrer Institute on the topic of diagnostics in the gas phase by laser-induced gratings (LIGs). The technique has been applied for thermometry in air and in flames at different pressures, for flow velocimetry, for concentration measurements, and for imaging purposes. The influence of collisional energy-transfer and relaxation processes in molecules on the temporal evolution of the LIG signals has also been investigated. It has been demonstrated that, for molecules with a low fluorescence quantum yield, excitation of laser-induced thermal gratings can be used as a sensitive spectroscopic tool. For the quantitative interpretation of the experiments shown in this work, the findings presented in the companion paper [1] have been used.     

Measurement of gas jet flow velocities using laser-induced electrostrictive gratings

We used time-resolved light scattering of cw probe laser radiation from laser-induced electrostrictive gratings for the determination of flow velocities in air at room temperature. Some possibilities of the technique have been experimentally demonstrated with submerged planar air jets in atmosphere, both for accumulated and single-shot measurements. The range of investigated flow velocities was 5–200 m/s. The method of data treatment and of the estimate of the experimental parameters is described. Received: 8 Febuary 2000 / Revised version: 2 May 2000 / Published online: 2 August 2000     

Gas phase diagnostics by laser-induced gratings I. theory

Electrostriction and collisional thermalization of absorbed laser energy are the two dominant mechanisms leading to the formation of laser-induced gratings (LIGs) in the gas phase. In this article the results of the theoretical investigations that have been achieved in the past ten years at the Paul Scherrer Institute on this issue are summarized and yield a comprehensive understanding of the underlying physical concepts. Furthermore, a study of the influence of various parameters, such as the alignment and the spatial intensity profile of the beams on the generated electrostrictive and thermal signal is presented for the first time to the authors’ knowledge. The variations of the refractive index responsible for the appearance of laser-induced gratings have been theoretically described by solving the linearized hydrodynamic equations. The contributions from electrostriction, as well as from instantaneous and slow relaxation of the absorbed radiation energy into heat is obtained. These expressions are employed for analysis of experimental data presented in the companion paper [1] which is devoted to the application of the technique for diagnostic purposes in the gas phase. Much effort has been undertaken in order to allow a straightforward physical interpretation of the experimental findings of the expressions presented here.     

Real-time measurements of trace gases using a compact difference-frequency-based sensor operating at 3.5 μm

3 for on-line absorption measurements of H₂CO, CH₄, and H₂O near 3.5 μm is reported. Formaldehyde levels of 30 ppb, corresponding to absorptions of 2×10^-4 have been measured using absorption spectroscopy. In this paper we report specifically the performance of this sensor as part of the 1997 Lunar–Mars Life Support Test program at the NASA Johnson Space Center. Received: 1 April 1998     

Spatio-temporal structure formation and self-diffraction in CdS using laser-induced thermal gratings

The semiconductor CdS is well known to show various kinds of photo-thermal and photo-electric optical nonlinearities. We present here to our knowledge first results of spatiotemporal structure formation using laser-induced thermal gratings in CdS. By the means of an optical multi-channel analyzer the spatial resolution of transverse dynamic switching processes was observed directly. Spatially and time resolved self-diffracted signals were measured in the far-field. The experimental results agree very well with calculations obtained by solving the heat-flow equation and using a fast Fourier transformation. The calculations verify the experimental parameters, in particular the thermal diffusivity D0.1 cm²/s at room temperature. To obtain a better transverse structuring, CdS samples were also investigated which were fixed on a sapphire substrate for longitudinal heat sinking.     

Structuring of aluminum films by laser-induced local oxidation in water

A simple method for patterning of thin (15–650 nm) aluminum films on glass substrates by direct, low-power, laser-thermal oxidation in water under common laboratory conditions is demonstrated. Local heating of the metal film enhances the formation of aluminum oxide (hydrargillite, Al₂O₃–3H₂O) and provokes breakdown of the passivation layer followed by local corrosion at temperatures close to the boiling point of water. Moving the focus of an Ar-ion laser (λ=488 nm) over the aluminum film with a speed of several μm/s yields grooves flanked by hydrargillite. Upon through oxidation of the metal these structures act as electrically insulating domains. Depending on the film thickness, the minimum width of the line structures measures between 266 nm and 600 nm. The required laser irradiation power ranges from 1.7 mW to 30 mW. It is found that the photo-thermal oxidation process allows for writing of two-dimensional electrode patterns. Received: 16 July 2001 / Accepted: 23 July 2001 / Published online: 2 October 2001     

Optical and microscopy investigations of soot structure alterations by laser-induced incandescence

2 at 1064 nm, vaporization/fragmentation of soot primary particles and aggregates occurs. Optical measurements are performed using a second laser pulse to probe the effects of these changes upon the LII signal. With the exception of very low fluences, the structural changes induced in the soot lead to a decreased LII intensity produced by the second laser pulse. These two-pulse experiments also show that these changes do not alter the LII signal on timescales less than 1 μs for fluences below the vaporization threshold. Received: 20 October 1997/Revised version: 16 February 1998     

Theoretical and experimental studies on laser-induced transient gratings in laser dyes

Laser-induced transient grating technique has been used to measure the diffraction efficiency (η) and calculate the third-order nonlinear susceptibility (χ⁽³⁾) of some laser dyes. Theoretical simulations have been carried out on η and χ⁽³⁾ as a function of wavelength covering the spectral range corresponding to the first excited singlet state of the dyes. Theoretically simulated values have been found in agreement to those observed experimentally. The decay profiles for these dyes have been measured by using diffraction of a delayed probe laser pulse to estimate the relaxation times in the excited state.     

Temperature and flow-velocity measurements by use of laser-induced electrostrictive gratings

Light scattering from laser-induced electrostrictive gratings has been used for simultaneous, instantaneous, nonintrusive, and remote measurements of temperature and velocity in a submerged air jet. We accomplished phase-sensitive detection of scattered light by superimposing two signal beams whose frequencies were Doppler shifted by the movement of the grating. Temperatures in the range 295-600 K and flow velocities in the range 10-100 m/s were measured.     

13CO2/12CO2 isotopic ratio measurements using a difference frequency-based sensor operating at 4.35 micrometers

A portable modular gas sensor for measuring the ¹³C/¹²C isotopic ratio in CO₂ with a precision of 0.8‰(±1σ) was developed for volcanic gas emission studies. This sensor employed a difference frequency generation (DFG)-based spectroscopic source operating at 4.35 μm (∼2300 cm^-1) in combination with a dual-chamber gas absorption cell. Direct absorption spectroscopy using this specially designed cell permitted rapid comparisons of isotopic ratios of a gas sample and a reference standard for appropriately selected CO₂ absorption lines. Special attention was given to minimizing undesirable precision degrading effects, in particular temperature and pressure fluctuations. Received: 16 April 2002 / Revised version: 28 May 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-713/5245237, E-mail: fkt@rice.edu     

Laser writing techniques for photomask fabrication using a femtosecond laser

Photomasks are the backbone of microfabrication industries. Currently they are fabricated by a lithographic process, which is very expensive and time consuming since it is a multi-step process. These issues can be addressed by fabricating photomasks by direct femtosecond laser writing, which is a single-step process and comparatively cheaper and faster than lithography. In this paper we discuss our investigations on the effect of two types of laser writing techniques, namely front- and rear-side laser writing, with regard to the feature size and the edge quality of a feature. It is proved conclusively that for the patterning of masks, front-side laser writing is a better technique than rear-side laser writing with regard to smaller feature size and better edge quality. Moreover the energy required for front-side laser writing is considerably lower than that for rear-side laser writing. Received: 22 May 2001 / Accepted: 14 September 2001 / Published online: 17 October 2001     

Soot volume fraction measurements in aero-engine exhausts using extinction-calibrated backward laser-induced incandescence

Control and reduction of soot particle emissions from aeronautic turbines requires a monitoring system suitable for quantification of these emissions. Currently, such emissions are estimated using the technique of smoke number. This is an extractive method, which is not sensitive enough for the low emission levels of modern gas turbines. Within a recent European project, AEROTEST, part of the project aimed at investigating an alternative soot monitoring technique, laser-induced incandescence (LII) as an in-situ optical diagnostic for quantification of soot emissions. For aero-engine applications, especially those involving large-scale turbines, it is necessary to perform the measurements at long distance from the turbine. The LII technique is favourable in this respect as it provides for non-intrusive measurements and, by detecting the isotropic LII signal along the same axis as the incoming laser beam (so called backward LII), both the laser and the detector can be built inside one system located several meters from the turbine. The concept was initiated in the previous European projects, AEROJET I and II. This paper describes the modified version of the system and the procedure developed to achieve reliable and quantitative soot volume fraction measurements in the exhausts of aero-engines. Application of the backward LII technique is demonstrated in the exhaust of a military turbojet engine for different engine speeds.     

Threshold reduction of stimulated Brillouin scattering (SBS) using fiber loop schemes

SBS mirrors as self-pumped and easy to handle non-linear optical devices are frequently used in high-power laser systems for improving the beam quality based on optical phase conjugation. Because of the non-linear behaviour, a certain pulse energy or power of incident light is needed to generate enough reflectivity for practical purposes. Therefore, reducing this “threshold” is still a main topic in the development of new schemes for optical phase conjugation. In addition to the taper concept reported earlier, this paper deals with loop schemes for reducing the power requirements. A reduction of the so-called “threshold” by a factor of between two and four was obtained with the schemes investigated using liquids and fibers. Received: 4 September 2001 / Revised version: 22 October 2001 / Published online: 23 November 2001     

Electric-field modulation measurements of complex electro-optic effects in poled polymer

Received: 10 July 1998/Revised version: 21 September 1998     

Beam-size effect in time-delayed laser-induced double gratings

We have studied theoretically the effect of the probe-beam size on time-delayed laser-induced double gratings by assuming that the probe beam is described as a Gaussian beam. LettingE _s1 andE _s2 be the Four-Wave Mixing (FWM) signals originating from the diffraction of the probe beam by the gratings, the condition for the occurrence of the FWM signal modulation is that the divergence angle ofE _s1 andE _s2 is larger than half of the intersection angle between the propagation directions ofE _s1 andE _s2. We have also proposed methods to increase the modulation contrast.     

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     

SBS pulse compression to 200 ps in a compact single-cell setup

Received: 14 September 1998 / Published online: 24 February 1999     

Broadly tunable difference-frequency spectrometer for trace gas detection with noncollinear critical phase-matching in LiNbO3

3 is reported. Using an external cavity diode laser, tunable from 795 to 825 nm, and a cw diode-pumped Nd:YAG ring laser at 1064 nm, we produced narrowband mid-ir laser light between 3.16 and 3.67 μm. This broad tuning range of 440 cm^-1 can be critically phase-matched by changing the external crystal angle within a range of only 0.4°. Even for a fixed crystal angle broadband phase-matching over 230 cm^-1 was achieved. No realignment was required when tuning the laser over the whole wavelength range, which enabled the use of a compact 36-m multipass cell as gas chamber. The conversion efficiency could be improved by almost a factor of 3 by applying noncollinear instead of collinear phase-matching, resulting in 30 nW of idler power with good beam quality. Spectra of methane were recorded in laboratory air, which demonstrate the rapid and continuous broad tunability at high sensitivity, enabling sub-ppm detection. Finally, wavelength modulation spectroscopy at high resolution was applied as a promising tool for further inproving the performance of this laser spectrometer. Received: 16 March 1998/Revised version: 1 July 1998     

Remote sensing of the atmosphere using ultrashort laser pulses

Theoretical and experimental studies were performed on the propagation of ultrashort optical terawatt pulses through the atmosphere. Propagation simulations of intense sub-picosecond pulses show that non-linear processes, such as white light generation, can be initiated at a chosen distance by selecting an appropriate group velocity dispersion. With this technique, a white light continuum was generated in the atmosphere whose spectral distribution was characterised in the visible and near infra-red. Applications of this novel light source for atmospheric remote sensing were investigated, combining lidar and time-resolved broadband absorption spectroscopy techniques. Measurements were performed on the oxygen molecule and water vapour. A comparison between the experimental results and the tabulated spectroscopic data led to an excellent correlation with measurements made on water vapour whereas observations on the oxygen showed discrepancy. This study demonstrates that the remote generation of a white light source represents a new way to access the range-resolved multi-trace gas analysis in the atmosphere. Received: 8 December 1999 / Revised version: 18 May 2000 / Published online: 16 August 2000