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Modulation transfer spectroscopy is used to demonstrate absolute frequency stabilization of an 8.6-µm-wavelength quantum cascade laser against a sub-Doppler absorption of the C H F 3 molecule. The obtained spectral emission properties are thoroughly characterized through a self-referenced optical frequency comb, stabilized against either a GPS-disciplined Rb clock or a 1.54-µm Er-fiber laser locked to a high-finesse ultra-low-expansion optical cavity. Fractional long-term stability and accuracy at a level of 4×10 -12 (at 100 s) and 3×10 -10 , respectively, are demonstrated, along with an emission linewidth as narrow as 10 kHz for observation times of 0.1 s.

We realized a UV laser spectrometer at 253.7 nm for Doppler broadening thermometry on the 1 S 0 - 3 P 1 intercombination line in mercury vapors. Our setup is based on the two-stage duplication of a 1014.8 nm diode laser in a fiber-coupled periodically poled lithium niobate waveguide crystal and a beta-barium borate crystal in enhancement cavity, and we exploit injection locking of a 507.4 nm diode laser to boost the available optical power after the first duplication. Our setup addresses spectroscopic features that allow the thermodynamic temperature determination of the atomic sample from the absorption profile with 10 -6 accuracy. The realized UV laser source has 1×10 -4 relative intensity stability, Gaussian shape, and over 10 GHz mode-hop-free tunable range. These features are crucial for the practical realization of the kelvin in the new International System of Units through a spectroscopic technique.

We report on absolute measurements of saturated-absorption line-center frequencies of room-temperature trifluoromethane using a quantum cascade laser at 8.6 μm and the frequency modulation spectroscopy method. Absolute calibration of the laser frequency is obtained by direct comparison with a mid-infrared optical frequency comb synthesizer referenced to a radio-frequency Rb standard. Several sub-Doppler transitions falling in the υ 5 vibrational band are investigated at around 1158.9  cm -1 with a fractional frequency precision of 8.6·10 -12 at 1-s integration time, limited by the Rb-clock stability. The demonstrated frequency uncertainty of 6.6·10 -11 is mainly limited by the reproducibility of the frequency measurements.

We developed a high-precision spectroscopic system at 8.6 μm based on direct heterodyne detection and phase-locking of a room-temperature quantum-cascade-laser against an harmonic, 250-MHz mid-IR frequency comb obtained by difference-frequency generation. The ∼30  dB signal-to-noise ratio of the detected beat-note together with the achieved closed-loop locking bandwidth of ∼500  kHz allows for a residual integrated phase noise of 0.78 rad (1 Hz-5 MHz), for an ultimate resolution of ∼21  kHz, limited by the measured linewidth of the mid-IR comb. The system was used to perform absolute measurement of line-center frequencies for the rotational components of the ν2 vibrational band of N2O, with a relative precision of 3×10(-10).

Frequency fluctuations of an optical frequency standard at 1.39 µm have been measured by means of a highly-sensitive optical frequency discriminator based on the fringe-side transmission of a high finesse optical resonator. Built on a Zerodur spacer, the optical resonator exhibits a finesse of 5500 and a cavity-mode width of about 120 kHz. The optical frequency standard consists of an extended-cavity diode laser that is tightly stabilized against the center of a sub-Doppler H(2) (18)O line, this latter being detected by means of noise-immune cavity-enhanced optical heterodyne molecular spectroscopy. The emission linewidth has been carefully determined from the frequency-noise power spectral density by using a rather simple approximation, known as β-line approach, as well as the exact method based on the autocorrelation function of the laser light field. It turns out that the linewidth of the optical frequency standard amounts to about 7 kHz (full width at half maximum) for an observation time of 1 ms. Compared to the free-running laser, the measured width corresponds to a line narrowing by a factor of ~220.

We report on a narrow-linewidth distributed-feedback quantum cascade laser at 8.6 μm that is optical-feedback locked to a high-finesse V-shaped cavity. The spectral purity of the quantum cascade laser is fully characterized using a high-sensitivity optical frequency discriminator, leading to a 1 ms linewidth of less than 4 kHz and a minimum laser frequency noise spectral density as low as 0.01 Hz2/Hz for Fourier frequencies larger than 100 kHz. The cumulative standard deviation of the laser intensity is better than 0.1% over an integration bandwidth from 2 Hz to 100 MHz.

We implemented an optical frequency standard based on noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) at 1.39 μm. The emission frequency of an extended-cavity diode laser was actively stabilized against the center of the 4(4,1)→4(4,0) transition of the H(2)(18)O ν1+ν3 band, under optical saturation conditions. The nonlinear regime of laser-gas interaction was reached by using an optical cavity with a finesse of about 8700. By filling it with an 18O-enriched water sample at a pressure of a few Pa, the Lamb dip could be observed with a full width at half-maximum of about 2 MHz. Absolute frequency stabilization was obtained by locking the cavity resonance to the center of the sub-Doppler signal, which was provided by the NICE-OHMS technique under the dispersion regime of operation. An Allan deviation analysis demonstrated a relative frequency stability of ∼5×10(-13) for an integration time of 1 s. For longer integration times, the flicker frequency noise floor set the stability at the level of 4×10(-14).

We demonstrate coherent phase locking of a room-temperature continuous-wave quantum cascade laser (QCL) at 9.1 μm to a Tm-fiber laser frequency comb centered at 2 μm, with an integrated residual phase error of 0.9 rad (30 mHz to 1.5 MHz). This resulted in a QCL linewidth reduction from 525 to 25 kHz at 1 ms observation time, limited by the linewidth of the free-running frequency comb.

This work presents a very simple yet effective way to obtain direct referencing of a quantum-cascade-laser at 4.3 μm to a near-IR frequency-comb. Precise tuning of the comb repetition-rate allows the quantum-cascade-laser to be scanned across absorption lines of a CO2 gaseous sample and line profiles to be acquired with extreme reproducibility and accuracy. By averaging over 50 acquisitions, line-centre frequencies are retrieved with an uncertainty of 30 kHz in a linear interaction regime. The extension of this methodology to other lines and molecules, by the use of widely tunable extended-cavity quantum-cascade-lasers, paves the way to a wide availability of high-quality and traceable spectroscopic data in the most crucial region for molecular detection and interrogation.

We describe a continuous-wave diode laser spectrometer for water-vapour precision spectroscopy at 1.38 μm. The spectrometer is based upon the use of a simple scheme for offset-frequency locking of a pair of extended-cavity diode lasers that allows to achieve unprecedented accuracy and reproducibility levels in measuring molecular absorption. When locked to the master laser with an offset frequency of 1.5 GHz, the slave laser exhibits residual frequency fluctuations of 1 kHz over a time interval of 25 minutes, for a 1-s integration time. The slave laser could be continuously tuned up to 3 GHz, the scan showing relative deviations from linearity below the 10{-6} level. Simultaneously, a capture range of the order of 1 GHz was obtained. Quantitative spectroscopy was also demonstrated by accurately determining relevant spectroscopic parameters for the 22,1→22,0line of the H2(18)O v1+v3 band at 1384.6008 nm.

We report the frequency stabilization of a cw extended-cavity diode laser against saturated absorption lines of the H(2)O17 isotopologue of water vapor at around 1.384 microm. The saturation of rotovibrational transitions is achieved by filling a high-finesse optical resonator with H(2)O17 at low pressure and by locking the laser frequency to the resonator by using the Pound-Drever-Hall technique. Absolute frequency stabilization is obtained, locking the cavity resonance to the center of the sub-Doppler line by means of the wavelength modulation method. A relative frequency stability of sigma(y)(tau)=10(-13)(0.1tau(-2)+0.9)(1/2) is demonstrated for integration times in the range 4 ms

The frequency of a DFB quantum cascade laser (QCL) emitting at 4.3 microm has been long-term stabilized to the Lamb-dip center of a CO2 ro-vibrational transition by means of first-derivative locking to the saturated absorption signal. Thanks to the non-linear sum-frequency generation (SFG) process with a fiber-amplified Nd:YAG laser, the QCL mid-infrared (IR) radiation has been linked to an optical frequency-comb synthesizer (OFCS) and its absolute frequency counted with a kHz-level precision and an overall uncertainty of 75 kHz.

A mid-infrared laser spectrometer was developed for simultaneous high-precision (18)O/(16)O and (17)O/(16)O isotope ratio measurements in carbon dioxide. A continuous-wave, liquid-nitrogen cooled, distributed feedback quantum cascade laser, working at a wavelength of 4.3 microm, was used to probe (12)C(16)O(2), (16)O(12)C(18)O, and (16)O(12)C(17)O lines at ~2311.8 cm(-1). High sensitivity was achieved by means of wavelength modulation spectroscopy with second-harmonic detection. The experimental reproducibility in the short and long terms was deeply investigated through the accurate analysis of a large number of spectra. In particular, we found a short term precision of 0.5 per thousand and 0.6 per thousand, respectively, for (18)O/(16)O and (17)O/(16)O isotope ratios. The occurrence of systematic deviations is also discussed.

We report what we believe to be the first absolute frequency measurement performed using a quantum-cascade laser (QCL) referenced to an optical frequency comb synthesizer (OFCS). A QCL at 4.43 microm has been used for producing near-infrared radiation at 858 nm by means of sum-frequency generation with a Nd:YAG source in a periodically poled lithium niobate nonlinear crystal. The absolute frequency of the QCL source has been measured by detecting the beat note between the sum frequency and a diode laser at the same wavelength, while both the Nd:YAG and the diode laser were referenced to the OFCS. Doppler-broadened line profiles of (13)CO(2) molecular transitions have been recorded with such an absolute frequency reference.

We report on the first application of extended-wavelength DFB diode lasers to Cavity-Enhanced Absorption Spectroscopy in-situ trace measurements on geothermal gases. The emission from the most active fumarole at the Solfatara volcano near Naples (Italy) was probed for the presence of CO and CH(4). After passing through a gas dryer and cooler, the volcanic gas flow (98% CO(2)) was analysed in real time for the concentration of these species, whose relatively strong absorption lines could be monitored simultaneously by a single Distributed Feed-Back (DFB) GaSb-based diode laser emitting around 2.33 mum (4300 cm(-1)) at room temperature. The concentrations were found to be about 3 ppm and 75 ppm, respectively, while actual detection limits for these molecules are around 1 ppb. We discuss the possibility of detecting other species of interest for volcanic emission monitoring.

We report the application of a cw distributed feedback quantum cascade laser to Lamb-dip spectroscopy of CO2 at 4.3 microm. With the laser operating in the free-running mode, we observed the sub-Doppler profile of the P(28) line of the (0,1(1),0)->(0,1(1),1) hot band by implementing a pump-probe scheme and using wavelength modulation spectroscopy for highly sensitive detection of saturated absorption signals. We investigated the main limitations to the observation of a narrow resonance, with particular attention to the effect of the laser current noise. We determined the intrinsic laser emission width, which was found to be approximately 3.4 MHz (FWHM) for an observation time of approximately 200 ms.

Carbon isotope ratio analysis using a laser-based technique has been performed in the field, on the gaseous emissions from an active volcano. We here describe that 13CO2/12CO2 determinations can be carried out in a quasi-continuous regime using a compact, selective and sensitive diode laser spectrometer at a wavelength of 2 mum. Within the Solfatara crater (near Naples, Italy), in a very harsh environment, we were able to determine relative 13CO2/12CO2 values, on the highest flux fumarole, with an accuracy of 0.5 per thousand. Regular and frequent observations of the carbon isotopes in volcanic gases, which become possible with our methodology, are of the utmost importance for geochemical surveillance of volcanoes.

A novel diode laser spectrometer was developed using dualwavelength multiplexing, ensuring ideal conditions for high-precision and simultaneous measurements of the 2H/1H, 17O/16O, and 18O/16O isotope ratios in water. A 1.4-m diode laser probed a H16OH / HO2H line pair near 7198 cm-1, while a similar laser observed H16OH, H17OH, and H18OH rovibrational lines around 7183 cm-1, or a H16OH / H18OH line pair near 7200 cm-1. The 1-sigma standard deviation is 0.2 per thousand for 18O/16O, and 0.5 per thousand for the 2H/1H and 17O/16O isotope ratios. Preliminary experiments with repeated injections of a natural abundance sample point to an accuracy of about 1 per thousand for all three isotope ratios in natural samples.

We reproduced the chemical-physical conditions of fumarolic emission at Phlaegrean Fields, Pozzuoli, Italy, and we measured the CO(2) and H(2)O concentrations using an absorption spectrometer based on two distributed feedback laser diodes at wavelengths of 1.578 and 1.393 microm. We discuss the accuracy levels of the different methods used. Furthermore, we measured the broadening coefficients for H(2)O (self-broadening, 28.2 +/- 0.6 MHz/Torr; CO(2) broadening, 6.0 +/- 0.4 MHz/Torr) and CO(2) (self-broadening, 3.2 +/- 0.1 MHz/Torr; H(2)O broadening, 4.0 +/- 0.1 MHz/Torr). Using the present data, we evaluated a minimum detectable variation of 9% for H(2)O and 1% for CO(2).

The Faraday effect was observed in the far-infrared spectrum of NO(2) for what is believed to be the first time. A systematic investigation of the magneto-optical signal as a function of the uncrossing angle between the polarizers was performed. Differences from similar experiments performed in the infrared and the visible regions were encountered. Moreover, a fit of the experimental data allowed calculation of the difference in the real and the imaginary terms of the refractive index for DM(F)=+1 and DM(F)=-1 multiplets.