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     

Laser frequency measurements and spectroscopic assignments of optically pumped 13CH3OH

A three-laser heterodyne system was used to measure the frequencies of twelve optically pumped laser emissions from ¹³CH₃OH in the far-infrared (FIR) region. These emissions, ranging from 54 to 142 μm, are reported with fractional uncertainties up to ±2×10^-7 along with their polarization relative to the CO₂ pump. Using the 9P32 and 10R14 CO₂ lines, complete spectroscopic assignments for two laser systems were confirmed. Received: 31 May 2001 / Published online: 19 September 2001     

Broadband difference frequency generation around 4.2 μm at overlapped phase-match conditions

Broadband difference frequency generation is theoretically and experimentally confirmed. It is shown that a wide tunable range of greater than 220 nm (FWHM) around 4.2 μm can be obtained in a 40 mm long periodically poled lithium niobate crystal with a single quasi-phase-matched period at a certain temperature. The broad bandwidth can be explained by means of the group-velocity matching or phase-mismatch minimization at overlapped phase-match conditions. The result shows that the broadband mid-infrared (mid-IR) laser source may find profound applications in trace gases detection of multiple atmospheric species and high resolution spectroscopy.     

High-power intracavity frequency doubling of a Ti:sapphire femtosecond oscillator

We demonstrate intracavity frequency doubling of a standard femtosecond Ti:sapphire oscillator. The cavity is extended with a pair of focusing mirrors and a 0.5-mm-thick BBO crystal. We achieve a repetition rate of 50 MHz and simultaneously generate 22 mW of 55-fs pulses at 810 nm and 200 mW of 73-fs pulses at 405 nm, which corresponds to 4 nJ per pulse. We create a total of 330-mW, 405-nm light when pumping the Ti:sapphire crystal with 5.7 W from an Ar-ion laser, corresponding to a conversion efficiency of 5.7%. No saturation is found, which implies that higher outputs can be achieved with higher pump rates. Preliminary results from the use of blue pulses as pump in an optical parametric amplifier seeded by pulses from a photonic crystal fiber are presented. Received: 27 January 2003 / Revised version: 27 March 2003 / Published online: 12 May 2003 RID="*" ID="*"Corresponding author. Fax: +45-861/96199, E-mail: tva@chem.au.dk     

Portable fiber-coupled diode-laser-based sensor for multiple trace gas detection

Tunable narrowband mid-infrared radiation from 3.25 to 4.4 μm is generated by a compact fiber-coupled, difference-frequency-based spectrosopic source. A 20-mW external cavity diode laser (with a tuning range from 814 to 870 nm) and a 50-mW distributed-Bragg-reflector diode-laser-seeded ytterbium-doped fiber amplifier operating at 1083 nm are difference-frequency mixed in a multi-grating, temperature-controlled periodically poled LiNbO₃ crystal. A conversion efficiency of 0.44 mW/(W² cm) (corresponding to a power of ≈3 μW at 3.3 μm) represents the highest conversion efficiency reported for a portable device. Performance characteristics of such a sensor and its application to spectroscopic detection of CO₂, N₂O, H₂CO, HCl, NO₂, and CH₄ will be reported in this work. Received: 14 May / Revised version: 24 June 1999 / Published online: 30 September 1999     

Chemical sensing with pulsed QC-DFB lasers operating at 15.6 micrometers

Pulsed thermoelectrically cooled QC-DFB lasers operating at 15.6 μm were characterized for spectroscopic gas sensing applications. A new method for wavelength scanning based on repetition rate modulation was developed. A non-wavelength-selective pyroelectric detector was incorporated in the sensor configuration giving the advantage of room-temperature operation and low cost. Absorption lines of CO₂ and H₂O were observed in ambient air, providing information about the concentration of these species. Received: 29 April 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-713/348-5686, E-mail: akoster@rice.edu     

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     

New short-wavelength laser emissions from partially deuterated methanol isotopes

The partially deuterated isotopes of methanol, CH₂DOH and CHD₂OH, have been reinvestigated as sources of far-infrared (FIR) laser emissions using an optically pumped molecular laser (OPML) system recently designed for wavelengths below 150 μm. With this system, 10 new FIR laser emissions from these isotopes ranging from 32.8 to 174.6 μm have been discovered. This includes the shortest known OPML emission from CHD₂OH, at 32.8 μm. These lines are reported with their operating pressure, polarizations relative to the CO₂ pump laser and wavelengths, measured to ±0.5 μm. In addition, polarizations for three previously observed FIR laser lines from CHD₂OH were measured for the first time. This paper is dedicated to the memory of Dr. K.M. Evenson, a pioneer in the field for his role in the development of optically pumped molecular lasers and their use in laser frequency measurements and the laser magnetic resonance technique. His scientific expertise, guidance, mentoring and friendship will be greatly missed. Received: 27 March 2002 / Published online: 8 May 2002     

Short-wavelength far-infrared laser cavity yielding new laser emissions in CD3OH

A significantly improved far-infrared laser has been used to generate optically pumped laser emissions from 26 to 150 μm for CD₃OH. Using an X–V-pumping geometry, several new laser emissions have been found for CD₃OH. In addition, an increase in power, by factors from 10 to 1000, for many of the previously known shorter-wavelength laser lines, below 100 μm, has been observed. Frequency measurements for several lines have also been performed and have been reported to a fractional uncertainty up to ±2×10^-7, permitting the spectroscopic assignment of the laser transition. One of the frequency-measured lines, 44.256 μm observed using the 10R34 pump, has confirmed the assignment of the previously reported FIR emission (n,K;J)=(1,7;20)?(0,8;20)A in the ground vibrational state. Received: 26 October 2000 / Published online: 7 February 2001     

Observation of iodine transitions using the second and third harmonics of a 1.5-μm laser

This paper presents spectroscopic measurements of iodine at 778 nm and 518 nm performed by second and third harmonics of a 1.5-μm diode laser, generated by quasi-phase matching in a periodically poled lithium niobate waveguide. Sub-Doppler spectroscopy by a 780-nm source was also demonstrated, and shows the potential of the system to reach high levels of frequency stability by locking the laser to the iodine transitions. The suggested method significantly improves the number of frequency references available for stabilizing 1550-nm lasers. Received: 4 February 2002 / Revised version: 14 May 2002 / Published online: 8 August 2002     

A laser system providing tunable, narrow-band radiation from 35 nm to 2 μm

We describe a laser system that readily provides radiation tunable from 2 μm in the infra-red to 35 nm in the extreme ultraviolet spectral range. The broad spectral range is covered through a range of non-linear processes such as Raman shifting and high-order harmonic generation. Pulses with duration of tens of picoseconds are obtained. The relative bandwidth of the radiation is δλ/λ=10^-4, comparable with what can be achieved by using high-resolution monochromators at state-of-the-art synchrotron beamlines. We discuss different methods for characterising the radiation in this wide wavelength regime. We also discuss the capabilities of the system from the measured parameters. Received: 12 December 2000 / Revised version: 8 March 2001 / Published online: 27 April 2001     

A dispersionless Michelson interferometer for the characterization of attosecond pulses

A novel application of a free-standing transmission grating as a beam splitter in a Michelson-type interferometer is described. The arrangement can operate in the XUV and soft X-ray spectral region and, therefore, it is well suited for the characterization of attosecond pulses. Using ray-tracing codes, we have analyzed three different setups in which spherical mirrors are employed in conjunction with the transmission grating and have investigated in detail their dispersive characteristics. It is shown that such an arrangement can be made to exhibit group-delay dispersion of ∼1 as² while it provides two co-propagating and converging beams. Received: 12 October 2001 / Revised version: 17 December 2001 / Published online: 7 February 2002     

Development of a tunable mid-IR difference frequency laser source for highly sensitive airborne trace gas detection

The development of a compact tunable mid-IR laser system at 3.5 μm for quantitative airborne spectroscopic trace gas absorption measurements is reported. The mid-IR laser system is based on difference frequency generation (DFG) in periodically poled LiNbO₃ and utilizes optical fiber amplified near-IR diode and fiber lasers as pump sources operating at 1083 nm and 1562 nm, respectively. This paper describes the optical sensor architecture, performance characteristics of individual pump lasers and DFG, as well as its application to wavelength modulation spectroscopy employing an astigmatic Herriott multi-pass gas absorption cell. This compact system permits detection of formaldehyde with a minimal detectable concentration (1σ replicate precision) of 74 parts-per-trillion by volume (pptv) for 1 min of averaging time and was achieved using calibrated gas standards, zero air background and rapid dual-beam subtraction. This corresponds to a pathlength-normalized replicate fractional absorption sensitivity of 2.5×10^-10 cm^-1. Received: 29 April 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-303/497-1492, E-mail: dr@ucar.edu     

Wavelength-modulation spectroscopy using a frequency-doubled current-modulated diode laser

We have studied atomic absorption in an argon discharge by wavelength-modulation spectroscopy with a frequency-doubled diode laser. The tunable wavelength-modulated radiation at 430 nm was generated by frequency doubling a current-modulated 860-nm diode laser in a KNbO₃ crystal. 2f-, 4f- and 6f-harmonic spectra as a function of diode laser modulation depth were measured on a Doppler-broadened sample of excited argon atoms produced in a capacitively coupled plasma chamber. Characterisation of the harmonic signals was accomplished. Minimum detectable absorbances of 7.7×10^-5 and 1.9×10^-4 based on a 3σ criterion (σ being the standard deviation of the noise) were estimated for 2f- and 4f-harmonic detection of the frequency-doubled radiation with a time constant of 0.1 s. The concentrations of argon in the 1s₄ state were found to be in the range of 3×10⁸ to 1.2×10¹¹ cm^-3 for the experimental conditions studied. Received: 25 February 2002 / Revised version: 4 April 2002 / Published online: 14 May 2002     

A laser system producing 5×1019 W/cm2 at 10 Hz

19 W/cm² have been achieved. Received: 10 March 1997/Revised version: 26 April 1997     

Bichromatic pulsed source in the visible and infrared

A source of bichromatic coherent radiation is described with independent tunability in wavelength, energy and pulse duration. The system is able to deliver pulses in the visible to infrared region with possible extension into the ultraviolet. Pulse durations can be tailored to be from 15 ps to 310 fs with collimated beam fluences of several mJ/cm². Received: 28 January 2002 / Revised version: 24 April 2002 / Published online: 12 July 2002     

Simultaneous detection of methane, oxygen and water vapour utilising near-infrared diode lasers in conjunction with difference-frequency generation

An all-diode-laser-based spectrometer is used for the simultaneous detection of methane, oxygen and water vapour. This is accomplished using a 760-nm diode laser and a 980-nm diode laser in conjunction with difference-frequency generation to 3.4 μm in a periodically poled lithium niobate crystal. Each of the output wavelengths is resonant with one of the molecular species. Simultaneous recordings over a 15-m open path of laboratory air are demonstrated. The recording scheme shows the wide applicability of a diode-laser-based difference-frequency spectrometer for the detection of molecular species in different wavelength ranges. By increasing the frequency of the 760-nm diode laser and decreasing the frequency of the 980-nm diode laser, a maximum continuous tuning range in the mid infrared of 3.6 cm^-1 is achieved. This enables the recording of several methane lines at atmospheric pressure. Pressure-dependence studies of methane lineshapes are also performed in an absorption cell. An indoor-air methane background level of 3 ppm is measured. The signal-to-noise ratio in the recorded methane spectra indicates that sub-ppm detection of methane at atmospheric pressure is feasible. Received: 6 March 2000 / Revised version: 19 June 2000 / Published online: 11 October 2000     

Fine tuning of the higher-order dispersion of a prismatic pulse compressor

The wavelength-dependent thermal refractive index gives an extra degree of freedom for adjustment of higher-order dispersion of a prismatic pulse compressor. The effect allows of fine tuning of both intracavity and extracavity dispersion of ultra-fast oscillators. The calculations have been carried out using a new and rather handy formalism, which describes the operation of a prism pulse compressor as a linear function of the ratio of the total glass path in the prisms and the prism apex distance. The validity of theoretical calculations is supported by experimental evidence. Received: 16 April 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +36-62/544658, E-mail: osvay@physx.u-szeged.hu     

Resonant generation of a difference harmonic at a quantized metallic film

Received: 20 September 1998 / Revised version: 27 January 1999     

Enhanced drilling using a dual-pulse Nd:YAG laser

A new method for improving the efficiency of laser drilling has been developed. Two synchronized free-running laser pulses from a tandem-head Nd:YAG laser are capable of drilling through 1/8-in-thick stainless-steel targets at a stand-off distance of 1 m without gas-assist. The combination of a high-energy laser pulse for melting with a properly tailored high-intensity laser pulse for liquid expulsion results in the efficient drilling of metal targets. We argue that the improvement in drilling is due to the recoil pressure generated by rapid evaporation of the molten material by the second laser pulse. Received: 29 August 2000 / Accepted: 18 December 2000 / Published online: 3 April 2001