Portable difference-frequency laser-based cavity leak-out spectrometer for trace-gas analysis

We report a portable mid-infrared spectrometer for trace-gas analysis which is based on an all-solid-state difference-frequency-generation laser. The spectrometer provides in situ absorption path lengths of more than 3 km by means of the cavity leak-out method, a cw variant of the cavity ring-down technique. The design, performance, and application of this spectrometer are presented. The light source utilizes difference-frequency generation in a periodically poled lithium niobate (PPLN) crystal pumped by two single-frequency solid-state lasers. A maximum power of 27 μW in the wavelength region near 3.3 μm is achieved using a pump power of 20 mW at 808 nm, a signal power of 660 mW at 1064 nm, and a 50-mm-long PPLN crystal. This corresponds to a conversion efficiency of 0.42 mW/(W² cm). We demonstrate that this portable laser system is suitable as a light source in a cavity leak-out spectrometer. We achieved a minimum detectable absorption coefficient of 1×10^-8/cm (integration time: 2 s), corresponding, for example, to a detection limit of 1 part per billion ethane. This compact trace-gas analyzer with high sensitivity and specificity is promising for various environmental and medical applications. Received: 8 April 2002 / Revised version: 28 May 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +49-211/811-3121, E-mail: muertz@uni-duesseldorf.de     

Trace-gas sensing in the 3.3-μm region using a diode-based difference-frequency laser photoacoustic system

A compact, diode-based difference-frequency laser system combined with a photoacoustic detection scheme is presented for trace-gas sensing. It features a broad, continuous tuning range (3.2–3.7 μm), a narrow line width (154 MHz), and room-temperature operation, and thus allows numerous gas species to be measured both isolated and in mixtures of different gases. Several trace-gas species of environmental interest were detected, and gas mixtures were analysed. The detection limits are in the low-ppmV range, e.g. 1.3 ppmV for methane, 1.8 ppmV for ethane, and 1.2 ppmV for hydrogen chloride. Received: 10 April 2002 / Revised version: 5 June 2002 / Published online: 12 September 2002 RID="*" ID="*"Corresponding author. Fax: +41-1/633-1077, E-mail: Sigrist@iqe.phys.ethz.ch     

Generation of 99-mW continuous-wave 285-nm radiation for magneto-optical trapping of Mg atoms

We have developed a tunable intense narrow-band 285 nm light source based on frequency doubling of 570 nm light in BBO. At input powers of 840 mW (including 130 mW used for locking purposes) we generate 99 mW UV radiation with an intensity profile suitable for laser-cooling experiments. The light is used for laser cooling of neutral magnesium atoms in a magneto-optical trap (MOT). We capture about 5×10⁶ atoms directly from a thermal beam and find that the major loss mechanism of the magnesium MOT is a near-resonant two-photon ionization process. Received: 15 February 2002 / Revised version: 13 August 2002 / Published online: 11 December 2002 RID="*" ID="*"Corresponding author. Fax: +45-4588/7762, E-mail: dnm@mic.dtu.dk Present address: Mikroelektronik Centret, Technical University of Denmark, Orsteds Plads, Bldg. 345 East, 2800 Kgs. Lyngby, Denmark     

The application of quasi-phase-matched parametric light sources to practical infrared chemical sensing systems

Quasi-phase-matched (QPM) materials allow the generation of spectroscopically useful infrared radiation in an efficient and broadly tunable format. Here, we describe several applications of QPM-based light sources to remote and local chemical sensing. The remote systems are gas imagers that employ a fiber-pumped continuous-wave optical parametric oscillator or a microlaser-pumped, diode-seeded optical parametric amplifier as the illumination source. Technology described for local sensing includes a cavity ring down spectrometer that employs a novel optical parametric generator–amplifier to achieve ≥350 cm^-1 of contiguous tuning and a long-wave infrared light source based on QPM GaAs. In each case the use of QPM materials in conjunction with effective pump sources instills simplicity and ruggedness into the sensing systems. Received: 15 April 2002 / Revised version: 6 June 2002 / Published online: 12 September 2002 RID="*" ID="*"Corresponding author. Fax: +1-925/294-2595, E-mail: tjkulp@sandia.gov RID="**" ID="**"Present address: Corning Inc., Corning, NY 14831, USA RID="*" ID="*"Present address: Corning Inc., Corning, NY 14831, USA RID="**" ID="**"Present address: Blue Leaf Networks, Sunnyvale, CA 94086, USA RID="***" ID="***"Present address: Sandia National Laboratories, Albuquerque, NM 87185, USA     

Phase-stabilized 4-fs pulses at the full oscillator repetition rate for a photoemission experiment

Compressing pulses of a mode-locked extended-cavity Ti:sapphire laser using a standard single-mode fiber and tilted-front-interface chirped mirrors yields phase-stabilized 4-fs, 3-nJ light pulses at the full, 24-MHz, repetition rate. The demonstrated source paves the way towards exploring interactions sensitive to the carrier-envelope-offset phase, such as, for example, photoemission from solid targets at moderate intensities (∼10¹² W/cm²). Received: 13 December 2002 / Published online: 26 February 2003 RID="*" ID="*"Corresponding author. Fax: +43-1/58801-38799, E-mail: apolonski@tuwien.ac.at     

Removal of oxygen atoms from a SiO2 surface by incoherent vacuum ultraviolet excimer irradiation

We have demonstrated the non-thermal removal of oxygen atoms from an oxidized silicon surface (SiO₂) on a silicon wafer by the use of a low-power (0.3 mW cm^-2) incoherent vacuum ultraviolet (VUV) light source at 126 nm. X-ray photoelectron spectroscopy (XPS) has shown that a maximum Si concentration of 80% appears at the surface after a 20-h irradiation with 9.8 eV photons, as a result of oxygen removal from the SiO₂ matrix. The surface morphology, however, indicates no damage or melting on the surface even after the irradiation. Received: 15 April 2002 / Accepted: 17 April 2002 / Published online: 10 September 2002 RID="*" ID="*"Permanent address: Nano-Tech Photon Inc., Shimotomita 4132-1, Shintomi, Miyazaki, 889-1404, Japan RID="**" ID="**"Corresponding author. Fax: +81-985/583-899, E-mail: kubodera@opt.miyazaki-u.jp     

Trace complex-molecule detection using near-IR diode lasers

The goal of the present paper was to develop an experimental technique to detect trace concentrations of complex molecules in the atmosphere using near-IR diode lasers. Ethanol and propane were chosen as model species. New optical, hardware, instrument-operation-mode and data-processing approaches for detection of trace complex molecules were developed. Different physical processes limiting the sensitivity of trace molecule detection were considered and solutions were developed to reduce the influence of these mechanisms on instrument operation. An absorption sensitivity of α_min=2.5×10^-5 for 4.5 ms measurement time was achieved, which is comparable with the sensitivity of “small” molecule detection. The first results utilizing this technique for in-field monitoring of trace complex molecules are presented. Received: 25 April 2002 / Revised version: 29 May 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +7-095/135-8281, E-mail: anber@nsc.gpi.ru     

Rapidly swept, continuous-wave cavity ringdown spectroscopy with optical heterodyne detection: single- and multi-wavelength sensing of gases

Spectroscopic sensing of gases can be performed with high sensitivity and photometric precision by cavity ringdown (CRD) absorption spectroscopy. Our cavity ringdown spectrometer incorporates continuous-wave (cw) tunable diode lasers, fibre-optic coupling and standard photonics and optical telecommunications components. It comprises a rapidly swept optical cavity in a single-ended optical heterodyne transmitter–receiver configuration, enabling optical absorption of gases to be recorded either as single-frequency scanned spectra or as simultaneous, multi-wavelength tailored spectra. By measuring weak near-infrared rovibrational spectra of carbon dioxide gas (CO₂), with high resolution in the vicinity of 1.53 μm, we have realised a noise-limited absorption sensitivity of 2.5×10^-9 cm^-1 Hz^-1/2. Analytical sensitivity limits (both actual and projected) and prospective gas-diagnostic applications are discussed. Our approach to cw-CRD spectroscopy offers high performance in a relatively simple, low-cost, compact instrument that is amenable to chemical analysis of trace gases in medical, agricultural, industrial and environmental situations. Received: 16 May 2002 / Revised version: 3 June 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +61-2/9850-8313, E-mail: brian.orr@mq.edu.au     

Loss-tolerant, narrow-band reflector in the UV using a grating-waveguide structure

We theoretically demonstrate the feasibility of using a grating-waveguide structure (GWS) as a loss-tolerant, narrow-band reflector in the UV. We simulate device operation using a Green-function technique. Our numerical simulations indicate that a GWS with a 25-nm grating can be used as a 95% reflector for 157-nm light, even in the presence of intensity absorptions of 50 cm^-1. Received: 23 July 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-551/5035-99, E-mail: mbader@llg.gwdg.de     

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     

Sensitive absorption measurements in the near-infrared region using off-axis integrated-cavity-output spectroscopy

A novel instrument that employs a high-finesse optical cavity as an absorption cell has been developed for sensitive measurements of gas mixing ratios using near-infrared diode lasers and absorption-spectroscopy techniques. The instrument employs an off-axis trajectory of the laser beam through the cell to yield an effective optical path length of several kilometers without significant unwanted effects due to cavity resonances. As a result, a minimum detectable absorption of approximately 1.4×10^-5 over an effective optical path of 4.2 km was obtained in a 1.1-Hz detection bandwidth to yield a detection sensitivity of approximately 3.1×10^-11 cm^-1 Hz^-1/2. The instrument has been used for sensitive measurements of CO, CH₄, C₂H₂ and NH₃. Received: 6 May 2002 / Revised version: 31 May 2002 / Published online: 2 September 2002 RID="*" ID="*"Corresponding author. Fax: +1-650/965-7074, E-mail: d.baer@lgrinc.com     

Electrooptic properties of lithium niobate crystals for extremely high external electric fields

The electrooptic effect in lithium niobate crystals (LiNbO₃) for extremely high externally applied electric fields of up to 65 kV/mm is investigated. Homogeneous electrooptic refractive-index changes of up to 4.8×10^-3 are found for ordinarily polarized light. No quadratic electrooptic effect is observed. An upper bound for the quadratic electrooptic coefficient of |s₁₃|≤2.3×10^-21 m²/V² is determined. Electrooptic, angular, and wavelength tuning of the Bragg condition of a thermally fixed hologram are demonstrated. Received: 29 October 2002 / Revised version: 14 January 2003 / Published online: 26 March 2003 RID="*" ID="*"Corresponding author. E-mail: ml@uni-bonn.de     

Differential Helmholtz resonant photoacoustic cell for spectroscopy and gas analysis with room-temperature diode lasers

The results of theoretical and experimental studies and the design of a multi-purpose differential Helmholtz resonant photoacoustic detector (DHRD) and its applications to high-resolution spectroscopy of molecular gases and gas analysis with a room-temperature diode laser in the near-IR region are summarized. The series of experiments and numerical analysis of the DHRD sensitivity were performed for both types (single-pass and multi-pass) of DHRDs within a wide pressure range 0.1–101 kPa, including the regime of a gas flowing through a DHRD cell. The hardware and electronic arrangement of DHRDs for diode laser spectrometers and gas analyzers providing a limiting absorption sensitivity better than 10^-7 Wm^-1 are described. The results of measurements of spectral line parameters of H₂O near 800 and 1390 nm and CH₄ near 1650 nm (intensities, line broadening and shifting by atomic and molecular gases) are presented and discussed. The problems and the ways of perfection of the methodology and accuracy of DHRD techniques with tunable diode lasers of near-IR and visible spectral ranges are discussed. Received: 1 April 2002 / Revised version: 20 June 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +7/382-225-8026, E-mail: kvan@asd.iao.ru     

Theory of optical bistability in a non-linear quasi-waveguide

Optical bistable behavior in a quasi-waveguide containing non-linear film has been experimentally investigated in several publications in the past years; however, the physical mechanism for optical bistability has not been theoretically explained. In the present letter, we propose a theoretical model and successfully explain the observed optical bistability of both the reflected light and the scattered light (m-lines) in a non-linear quasi-waveguide. The optical bistability in the non-linear quasi-waveguide is due to the scattering-type wavevector mismatch mechanism. Received: 10 July 2002 / Revised version: 10 September 2002 / Published online: 20 December 2002 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: htwang@nju.edu.cn     

Generation of 100 μJ pulses at 82.8 nm by frequency tripling of sub-picosecond KrF laser radiation

. Investigations of the efficient generation of powerful coherent radiation at 82.8 nm by frequency tripling of short-pulse KrF laser radiation are presented. Argon gas is selected as nonlinear medium due to the resonantly enhanced 3rd-order susceptibility χ⁽³⁾(-3ω,ω,ω,ω). Pulse energies of 100 μJ at 82.8 nm have been measured for a pump pulse energy of 14 mJ. An upscaling to more than 500 μJ is expected with available more powerful pump lasers. Features of this XUV source and possible applications are discussed. Received: 26 July 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-511/7622211, E-mail: reinhardt@iqo.uni-hannover.de     

Power-boosted difference-frequency source for high-resolution infrared spectroscopy

We analyzed the spectroscopic performance of a difference-frequency source that utilizes a 5-W Yb-fiber amplifier for the “signal” radiation in order to increase the “idler” power generated around 4.3 μm. The amplifier is seeded by a monolithic-cavity Nd:YAG laser at 1064 nm. The intensity noise spectral density of the “idler” radiation was characterized. Cavity-enhanced saturated-absorption spectroscopy was also performed to test the frequency resolution. In particular, we observed the Lamb-dip spectrum of the ro-vibrational (00⁰0-00⁰1)R(0)transition of ¹⁷O¹²C¹⁶O in natural abundance. To our knowledge, this is the first observation of that transition by the Lamb-dip technique. Received: 19 December 2002 / Revised version: 3 February 2003 / Published online: 16 April 2003 RID="*" ID="*"Corresponding author. Fax: +39-055/4572-451, E-mail: mazzotti@inoa.it     

High-peak-power diode-pumped passively Q-switched Nd:YVO<Subscript>4</Subscript> laser

We report on a passively Q-switched diode-pumped Nd:YVO₄ laser polarized along the a axis (corresponding to the smallest value of emission cross section at 1064 nm), generating 157-μJ pulses with 6.0-ns time duration (>20 kW peak power) and 3.6 W of average power at 1064 nm with good beam quality (M²<1.4). The selection of the polarization was performed by a novel technique relying on the birefringence of the laser crystal and on the misalignment sensitivity of the resonator. Received: 30 September 2002 / Revised version: 22 November 2002 / Published online: 19 March 2003 RID="*" ID="*"Corresponding author. Fax: +39-382/422583, E-mail: agnesi@ele.unipv.it     

Three-dimensional structuring of sapphire by sequential He+ ion-beam implantation and wet chemical etching

We present a method for the selective two- and three-dimensional patterning of sapphire using light ion-beam implantation to generate severe lattice damage to depths exceeding 1 μm and subsequent selective wet chemical etching of the damaged regions by hot H₃PO₄. C-cut sapphire crystals were implanted through contact masks using ion fluences of 1×10¹⁶ to 5×10¹⁷ He⁺/cm² and energies up to 400 keV. The etching process is characterized by a high selectivity and a rate of approximately 19 nm/min. Whereas an implantation that produces a continuously damaged pathway results in complete etching from the surface, sole in-depth implantation using only high-energy ions leads to under-etching of the crystalline surface layer. By a combination of these processes we have fabricated three-dimensional structures such as channels and bridges in sapphire. Received: 14 October 2002 / Accepted: 15 October 2002 / Published online: 26 February 2003 RID="*" ID="*"Corresponding author. Fax +41-21/693-3701, E-mail: aurelian.crunteanustanescu@epfl.ch     

In situ synthesis of mesoporous CdS nanoparticles in ternary cubic phase lyotropic liquid crystal

An in situ technique for the synthesis of CdS nanoparticles in a ternary lyotropic cubic phase liquid crystal has been carried out. The extremely viscous cubic phase liquid-crystal system consists of poly(oxyethylene)₁₀ nonyl phenol ether as non-ionic surfactant, octane as oil phase and an aqueous phase containing reactant ions (Cd²⁺ and S^2-). Thioacetamide (TAA) has been utilized as a source for slow release of sulfur in the in situ synthesis of CdS. Rheological results show that CdS nanoparticle growth did not disrupt the structure of the cubic phase liquid-crystal system. This indicates that homogenous synthesis of CdS in the liquid crystal had been achieved. The final products were characterized using X-ray photoelectron spectroscopy, thermal gravimetric analysis, transmission electron microscopy and UV-visible spectroscopy. It was found that the CdS nanoparticles formed have a mesoporous structure with a size dependent on the TAA decomposition aging time. Received: 29 March 2002 / Accepted: 4 September 2002 / Published online: 17 December 2002 RID="*" ID="*"Corresponding author. Fax: +603-8921/3257, E-mail: shahidan@pkrisc.cc.ukm.my     

A fast-response near-infrared tunable diode laser absorption spectrometer for in situ measurements of CH4 in the upper troposphere and lower stratosphere

We describe a near-infrared in situ tunable diode laser spectrometer developed for atmospheric measurements of CH₄ in the upper troposphere and lower stratosphere (UT/LS). The instrument is designed to provide fast-response (0.5–1 Hz) measurements and operate autonomously on the NASA WB-57F high-altitude aircraft. A single-mode InGaAsP distributed feedback laser diode operating at 1.6537 μm scans continuously over the R(3) rotation–vibration transition in the 2ν₃ band. We use a direct absorption technique incorporating a custom-designed long path length (252 m) low-volume (3.6 L) astigmatic Herriott cell. The present detection sensitivity is 5×10¹⁰ molecules cm^-3, corresponding to ∼20 ppbv in the UT/LS, with the main limit to instrument precision being background optical interference fringes. In-flight performance is demonstrated by presentation of recent data. Received: 25 January 2002 / Revised version: 5 April 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-303/497-5373, E-mail: richard@al.noaa.gov