Free-running frequency stability of mid-infrared quantum cascade lasers.

The intrinsic frequency fluctuations of two single-mode quantum cascade (QC) distributed-feedback lasers operating continuously at a wavelength of 8.5 mum are reported. A Doppler-limited rovibrational resonance of nitrous oxide is used to transform the frequency noise into measurable intensity fluctuations. The QC lasers, along with recently improved current controllers, exhibit a free-running frequency stability of 150 kHz over a 15-ms time interval.

Quantum-cascade laser measurements of stratospheric methane and nitrous oxide.

A tunable quantum-cascade (QC) laser has been flown on NASA's ER-2 high-altitude aircraft to produce the first atmospheric gas measurements with this newly invented device, an important milestone in the QC laser's future planetary, industrial, and commercial applications. Using a cryogenically cooled QC laser during a series of 20 aircraft flights beginning in September 1999 and extending through March 2000, we took measurements of methane (CH(4)) and nitrous oxide (N(2)O) gas up to ~20 km in the stratosphere over North America, Scandinavia, and Russia. The QC laser operating near an 8-mum wavelength was produced by the groups of Capasso and Cho of Bell Laboratories, Lucent Technologies, where QC lasers were invented in 1994. Compared with its companion lead salt diode lasers that were also flown on these flights, the single-mode QC laser cooled to 82 K and produced higher output power (10 mW), narrower laser linewidth (17 MHz), increased measurement precision (a factor of 3), and better spectral stability (~0.1 cm(-1) K). The sensitivity of the QC laser channel was estimated to correspond to a minimum-detectable mixing ratio for methane of approximately 2 parts per billion by volume.

Application of Balanced Detection to Absorption Measurements of Trace Gases with Room-Temperature, Quasi-cw Quantum-Cascade Lasers.

Distributed-feedback quantum-cascade (QC) lasers are expected to form the heart of the next-generation mid-IR laser absorption spectrometers, especially as they are applied to measurements of trace gases in a variety of environments. The incorporation of room-temperature-operable, single-mode QC lasers should result in highly compact and rugged sensors for real-world applications. We report preliminary results on the performance of a laser absorption spectrometer that uses a QC laser operating at room temperature in a quasi-cw mode in conjunction with balanced ratiometric detection. We have demonstrated sensitivities for N(2)O [10 parts in 10(6) volume-mixing ratio for a 1-m path (ppmv-m)] and NO [520 parts in 10(9) volume-mixing ratio for a 1-m path (ppbv-m)] at 5.4 mum. System improvements are described that are expected to result in a 2 orders of magnitude increase in sensitivity.

Cavity ringdown spectroscopic detection of nitric oxide with a continuous-wave quantum-cascade laser.

A spectroscopic gas sensor for nitric oxide (NO) detection based on a cavity ringdown technique was designed and evaluated. A cw quantum-cascade distributed-feedback laser operating at 5.2 mum was used as a tunable single-frequency light source. Both laser-frequency tuning and abrupt interruptions of the laser radiation were performed through manipulation of the laser current. A single ringdown event sensitivity to absorption of 2.2 x 10(-8) cm(-1) was achieved. Measurements of parts per billion (ppb) NO concentrations in N(2) with a 0.7-ppb standard error for a data collection time of 8 s have been performed. Future improvements are discussed that would allow quantification of NO in human breath.

Spectroscopic detection of biological NO with a quantum cascade laser.

Two configurations of a continuous wave quantum cascade distributed feedback laser-based gas sensor for the detection of NO at a parts per billion (ppb) concentration level, typical of biomedical applications, have been investigated. The laser was operated at liquid nitrogen temperature near lambda = 5.2 microns. In the first configuration, a 100 m optical path length multi-pass cell was employed to enhance the NO absorption. In the second configuration, a technique based on cavity-enhanced spectroscopy (CES) was utilized, with an effective path length of 670 m. Both sensors enabled simultaneous analysis of NO and CO2 concentrations in exhaled air. The minimum detectable NO concentration was found to be 3 ppb with a multi-pass cell and 16 ppb when using CES. The two techniques are compared, and potential future developments are discussed.

Absorption spectroscopy with quantum cascade lasers.

Novel pulsed and cw quantum cascade distributed feedback (QC-DFB) lasers operating near lambda=8 micrometers were used for detection and quantification of trace gases in ambient air by means of sensitive absorption spectroscopy. N2O, 12CH4, 13CH4, and different isotopic species of H2O were detected. Also, a highly selective detection of ethanol vapor in air with a sensitivity of 125 parts per billion by volume (ppb) was demonstrated.

Self-mode-locking of quantum cascade lasers with giant ultrafast optical nonlinearities.

We report on the generation of picosecond self-mode-locked pulses from midinfrared quantum cascade lasers, at wavelengths within the important molecular fingerprint region. These devices are based on intersubband electron transitions in semiconductor nanostructures, which are characterized by some of the largest optical nonlinearities observed in nature and by picosecond relaxation lifetimes. Our results are interpreted with a model in which one of these nonlinearities, the intensity-dependent refractive index of the lasing transition, creates a nonlinear waveguide where the optical losses decrease with increasing intensity. This favors the generation of ultrashort pulses, because of their larger instantaneous intensity relative to continuous-wave emission.

Effective utilization of quantum-cascade distributed-feedback lasers in absorption spectroscopy.

A variable duty cycle quasi-cw frequency scanning technique was applied to reduce thermal effects resulting from the high heat dissipation of type I quantum-cascade lasers. This technique was combined with a 100-m path-length multipass cell and a zero-air background-subtraction technique to enhance detection sensitivity to a parts-in-10(9) (ppb) concentration level for spectroscopic trace-gas detection of CH4, N2O, H2O, and C2H5OH in ambient air at 7.9 micrometers. A new technique for analysis of dense high resolution absorption spectra was applied to detection of ethanol in ambient air, yielding a 125-ppb detection limit.

High-power, continuous-wave, current-tunable, single-mode quantum-cascade distributed-feedback lasers at lambda - 5.2 and lambda - 7.95 mum.

Quantum-cascade distributed-feedback lasers with high-power, continuous-wave (cw), tunable, single-mode emission are reported. The emission wavelengths are near 5.2 and 7.95 mum. The lasers are operated at liquid-nitrogen temperature and above. A maximum output power of >100 mW is obtained per facet at 80 K for both wavelengths, which is the result of careful positioning of the peak gain with respect to the Bragg wavelength. Continuous tuning with either heat-sink temperature or cw current is demonstrated. The tuning coefficients are 0.35 nm/K (5.2 mum) and 0.51 nm/K(7.95 mum) for thermal tuning and vary from 20 to 40 nm/A for tuning with current. The lasers are being used in high-resolution and high-sensitivity gas-sensing applications.

Cavity ringdown spectroscopy using mid-infrared quantum-cascade lasers.

Cavity ringdown spectra of ammonia at 10 parts in 10(9) by volume (ppbv) and higher concentrations were recorded by use of a 16-mW continuous-wave quantum-casacde distributed-feedback laser at 8.5 mum whose wavelength was continuously temperature tuned over 15 nm. A sensitivity (noise-equivalent absorbance) of 3.4x10(-9) cm(-1) Hz(-1/2) was achieved for ammonia in nitrogen at standard temperature and pressure, which corresponds to a detection limit of 0.25 ppbv.

Quantitative gas sensing by backscatter-absorption measurements of a pseudorandom code modulated lambda ~ 8-microm quantum cascade laser.

We have demonstrated quantitative chemical vapor detection with a multimode quantum cascade (QC) laser. Experiments incorporated pseudorandom code (PRC) modulation of the laser intensity to permit sensitive absorption measurements of isopropanol vapor at 8.0micro . The demonstration shows the practicality of one technical approach for implementing low-peak-power QC lasers in the transmitter portion of a differential absorption lidar (DIAL) system. With a 31-chip, 300-ns/chip PRC sequence, the measured isopropanol detection limit was 12 parts in 10(6) by volume times meters (~3x10(-3) absorption) for a simple backscatter-absorption measurement configuration.

Trace-gas detection in ambient air with a thermoelectrically cooled, pulsed quantum-cascade distributed feedback laser.

A pulsed quantum-cascade distributed feedback laser operating at near room temperature was used for sensitive high-resolution IR absorption spectroscopy of ambient air at a wavelength of approximately 8 microm. Near-transform-limited laser pulses were obtained owing to short (approximately 5-ns) current pulse excitation and optimized electrical coupling. Fast and slow computer-controlled frequency scanning techniques were implemented and characterized. Fast computer-controlled laser wavelength switching was used to acquire second-derivative absorption spectra. The minimum detectable absorption was found to be 3 x 10(-4) with 10(5) laser pulses (20-kHz repetition rate), and 1.7 x 10(-4) for 5 x 10(5) pulses, based on the standard deviation of the linear regression analysis.

Methane concentration and isotopic composition measurements with a mid-infrared quantum-cascade laser.

A quantum-cascade laser operating at a wavelength of 8.1 micrometers was used for high-sensitivity absorption spectroscopy of methane (CH4). The laser frequency was continuously scanned with current over more than 3 cm-1, and absorption spectra of the CH4 nu 4 P branch were recorded. The measured laser linewidth was 50 MHz. A CH4 concentration of 15.6 parts in 10(6) ( ppm) in 50 Torr of air was measured in a 43-cm path length with +/- 0.5-ppm accuracy when the signal was averaged over 400 scans. The minimum detectable absorption in such direct absorption measurements is estimated to be 1.1 x 10(-4). The content of 13CH4 and CH3D species in a CH4 sample was determined.

Photoacoustic spectroscopy using quantum-cascade lasers.

Photoacoustic spectra of ammonia and water vapor were recorded by use of a continuous-wave quantum-cascade distributed-feedback (QC-DFB) laser at 8.5 mum with a 16-mW power output. The gases were flowed through a cell that was resonant at 1.6 kHz, and the QC-DFB source was temperature tuned over 35 nm for generation of spectra or was temperature stabilized on an absorption feature peak to permit real-time concentration measurements. A detection limit of 100 parts in 10(9) by volume ammonia at standard temperature and pressure was obtained for a 1-Hz bandwidth in a measurement time of 10 min.

Kilohertz linewidth from frequency-stabilized mid-infrared quantum cascade lasers.

Frequency stabilization of mid-IR quantum cascade (QC) lasers to the kilohertz level has been accomplished by use of electronic servo techniques. With this active feedback, an 8.5-microm QC distributed-feedback laser is locked to the side of a rovibrational resonance of nitrous oxide (N(2) O) at 1176.61cm (-1) . A stabilized frequency-noise spectral density of 42Hz/ radicalHz has been measured at 100 kHz; the calculated laser linewidth is 12 kHz.

High-resolution (Doppler-limited) spectroscopy using quantum-cascade distributed-feedback lasers.

Lasing characteristics were evaluated for distributed-feedback quantum-cascade (QC) lasers operating in a continuous mode at cryogenic temperatures. These tests were performed to determine the QC lasers' suitability for use in high-resolution spectroscopic applications, including Doppler-limited molecular absorption and pressure-limited lidar applications. By use of a rapid-scan technique, direct absorbance measurements of nitric oxide (NO) and ammonia (NH>(3)) were performed with several QC lasers, operating at either 5.2 or 8.5 microm. Results include time-averaged linewidths of better than 40 MHz and long-term laser frequency reproducibility, even after numerous temperature cycles, of 80 MHz or better. Tuning rates of 2.5 cm(-1) in 0.6 ms can be easily achieved. Noise-equivalent absorbance of 3 x 10(-6) was also obtained without optimizing the optical arrangement.