Design considerations in high-sensitivity off-axis integrated cavity output spectroscopy

Off-axis integrated cavity output spectroscopy (OA-ICOS) has generated much interest because it potentially allows highly sensitive field measurements with robust optical alignment. We discuss here design choices involved in design of an OA-ICOS instrument and how these choices impact instrument sensitivity, using as our example the design of the Harvard ICOS isotope instrument, which demonstrates the highest reported sensitivity for mid-IR OA-ICOS (2.4×10^-11 cm^-1Hz^-1/2 at 6.7 μm, obtained during measurements of water vapor isotopologues H₂O, HDO, and H₂  ¹⁸O in the laboratory and onboard NASA’s WB-57 high-altitude research aircraft). We compare the sensitivity of several OA-ICOS instruments with differing design parameters, show how comparisons are hindered by differing definitions of instrument performance metrics, and suggest a common metric of MDA_meas, the fractional absorption equivalent to 1σ uncertainty in an actual measurement, normalized to 1 s integration. We also note that despite an emphasis on sensitivity in the literature, in the Harvard ICOS isotope instrument and likely also similar instruments, systematic errors associated with fitting of the baseline laser power are of equal importance to total measurement uncertainty.     

Optimum signal-to-noise ratio in off-axis integrated cavity output spectroscopy

The signal-to-noise ratio (SNR) in off-axis integrated cavity output spectroscopy (OA-ICOS) is investigated and compared to direct absorption spectroscopy using multipass absorption cells [tunable diode laser absorption spectroscopy (TDLAS)]. Applying measured noise characteristics of a near-IR tunable diode laser and detector, it is shown that the optimum SNR is not generally reached at the highest effective absorption path length. Simulations are used to determine the parameters for maximized SNR of OA-ICOS.     

Wavelength modulated off-axis integrated cavity output spectroscopy in the near infrared

A novel instrument based on an improved off-axis alignment of integrated cavity output spectroscopy (OA-ICOS) in conjunction with a wavelength modulation (WM) technique, was developed using a DFB diode laser operating in the near infrared at 1.573 μm (6357.3 cm^-1). The laser-based sensor employed a 44 cm optical cavity that provided an effective absorption path length of ∼68 m. A minimum detectable absorption of approximately 3.6 ppmv Hz^-1/2 or 2.3×10^-7 Hz^-1/2 per optical pass was obtained using second harmonic detection. We demonstrated that by implementation of the WM technique to OA-ICOS in the near infrared, the detection sensitivity was improved by a factor of 14 compared to that obtained with OA-ICOS. Measurements of CO₂ mixing ratios in ambient air have been performed by using both OA-ICOS and WM-OA-ICOS techniques for performance comparison. PACS 42.62.Fi; 07.07.Df; 33.20.Ea     

Detection of formaldehyde using off-axis integrated cavity output spectroscopy with an interband cascade laser

A continuous-wave, mid-infrared, distributed feedback, interband cascade laser was used to detect and quantify formaldehyde (H₂CO) using off-axis, integrated cavity output spectroscopy in gas mixtures containing ≈1–25 parts in 10⁶ by volume (ppmV) of H₂CO. Analysis of the spectral measurements indicates that a H₂CO concentration of 150 parts in 10⁹ by volume (ppbV) would produce a spectrum with a signal to noise ratio of 3 for a data acquisition time of 3 s. This is a relevant sensitivity level for formaldehyde monitoring of indoor air, occupational settings, and on board spacecraft in long duration missions in particular as the detection sensitivity improves with the square root of the data acquisition time. PACS 07.07.Df; 82.80.Ch     

H2S trace concentration measurements using off-axis integrated cavity output spectroscopy in the near-infrared

Hydrogen sulfide (H₂S) trace detection has been performed by means of a DFB diode laser-based off-axis integrated cavity output spectroscopy (OA-ICOS) near 1571.6 nm. A minimum detectable concentration of 670 ppb (3σ) for a 2 s averaging time was obtained with an effective optical pathlength of ∼1.8 km. PACS 07.07.Df; 33.20.Ea; 42.62.Fi; 82.80.Gk     

Study of gas detection based on integrated cavity output spectroscopy

A trace gases detection system based on integrated cavity output spectroscopy (ICOS) was developed, where a NIR tunable diode laser (TDL) was used as light source, an optical cavity composed by two plan-concave mirrors with reflection near 99.7% was used as the absorption cell. Trace water vapour (H₂O), carbon dioxide (CO₂), methane (CH₄), carbon monoxide (CO) and mixture of CO₂ and CO were tested by ICOS based on the characteristics absorption. The wavelength calibration, cavity transmission characteristics, quantitative measurement ability and sensitivity of the TDL-ICOS were also studied, and a evaluated minimum detectable sensitivity of 1.15 × 10^?7 cm^?1 was obtained when the system was used to CH₄ detection. The experiment results show that TDL-ICOS is expected to be a reliable and promising system for the detection of trace gases since it has some advantages such as real-time monitoring, simple device, easy operation, high sensitivity, good stability and quantitative ability.     

The study of wavelength modulation off-axis integrated cavity output spectroscopy in the case of Lorentzian absorption profile

According to the property of optical cavity and the principle of signals and systems, the mathematical derivations for wavelength modulation off-axis integrated cavity output spectroscopy (WM-OA-ICOS) are presented. And based on the analytical method, the function expression of WM-OA-ICOS signal from Lorentzian absorption profile is obtained. To validate the analyses and deductions, some special cases in 2f-harmonic detection of WM-OA-ICOS are studied and experimented with a built compact WM-OA-ICOS apparatus. It is found that the measured results can coincide with the deduced conclusions. The works can provide some references for the application of WM-OA-ICOS in the case of Lorentzian absorption profile.     

Off-axis integrated cavity output spectroscopy and its application

Based upon the property of optical cavity and the principle of signals and systems, the measural theory and signal expression of off-axis integrated cavity output spectroscopy (Off-axis ICOS) have been analyzed and deduced. A compact and low-cost Off-axis ICOS apparatus, which used a special circuit to integrate the cavity output signal, was then described and experimented. The absorption spectrum of water vapor in the spectral range of 6587∼6595.5 cm⁻¹ was measured with this Off-axis ICOS system, and the measured spectral parameters were compared with the results of continuous-wave cavity ring down spectroscopy (CW-CRDS) and HITRAN2004 database. The detectable sensitivity of the system was achieved as ∼2.8 × 10⁻⁹ cm⁻¹.     

Ultra-sensitive mid-infrared cavity leak-out spectroscopy using a cw optical parametric oscillator

We report a portable, all-solid-state, mid-infrared spectrometer for trace-gas analysis. The light source is a continuous-wave optical parametric oscillator based on PPLN and pumped by a Nd:YAG laser at 1064 nm. The generated single-frequency idler output covers the wavelength region between 2.35 and 3.75 μm. With its narrow line width, this light source is suitable for precise trace-gas analysis with very high sensitivity. Using cavity leak-out spectroscopy we achieved a minimum detectable absorption coefficient of 1.2×10^-9 /cm (integration time: 16 s), corresponding, for example, to a detection limit of 300 parts per trillion ethane. This sensitivity and the compact design make this trace-gas analyzer a promising tool for various in situ environmental and medical applications. Received: 19 September 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-228/733-474, E-mail: frank.kuehnemann@iap.uni-bonn.de     

Off-axis re-entrant cavity ring-down spectroscopy with a mid-infrared continuous-wave optical parametric oscillator

We demonstrate an off-axis cavity ring-down spectroscopy system, which uses a mid-infrared continuous-wave optical parametric oscillator as a light source. Off-axis injection with re-entrant configuration of the ring-down cavity is used to achieve high spectral resolution while maintaining high measurement speed. This makes the setup suitable for sensitive molecular spectroscopy in the mid-infrared region, particularly for studies that require high temporal resolution. Formaldehyde (H₂CO) absorption spectrum at 3.4 µm is measured using the off-axis re-entrant cavity ring-down spectrometer.     

Optical parametric oscillator on dipolaritons

The dynamics of dipolariton states in a planar microcavity under pumping into the middle dipolariton branch is investigated. It is shown that, in the case of exact resonance, the system exhibits an aperiodic behavior whereby pump dipolaritons are converted into dipolaritons of the idler and signal modes.     

Optical parametric oscillator based on four-wave mixing in microstructure fiber

We demonstrate, for the first time to our knowledge, optical parametric oscillation based on four-wave mixing in microstructure fiber. The measured wavelength-tunability range of the device (40 nm) and the threshold-pump peak power (34.4 W) are in good agreement with the theory of four-wave mixing in optical fibers. The ellipticity of the fiber's polarization modes allows the device to be implemented in a relatively simple Fabry-Perot configuration. Spectral peaks that are due to cascaded-mixing processes are easily observed in our setup, which may provide a way to extend the tunability range of existing high-power lasers.     

Wavelength-swept optical parametric oscillator for broadband mid-infrared spectroscopy

In this work we describe a wavelength-swept continuous-wave optical parametric oscillator (OPO) for the rapid acquisition of mid-infrared spectra spanning over hundreds of wavenumbers. Rapid tuning of a ytterbium-doped fibre pump laser resulted in the OPO idler tuning over 900 cm^?1 in 3.36 ms at a resolution of 4.5 cm^?1, within a total accessible range of 2.67 to 4.34 μm (2304–3752 cm^?1). Predictable tuning characteristics allowed simple online calibration of recorded spectra for absolute mid-infrared frequency. The system thus offers a viable approach to broadband spectral acquisition in applications requiring high-radiance illumination.     

Quantum cascade laser-based integrated cavity output spectroscopy of exhaled nitric oxide

A nitric oxide (NO) sensor employing a thermoelectrically cooled, continuous-wave, distributed feedback quantum cascade laser operating at 5.47 μm (1828 cm^-1) and off-axis integrated cavity output spectroscopy was used to measure NO concentrations in exhaled breath. A minimum measurable concentration (3σ) of 3.6 parts-per-billion by volume (ppbv) of NO with a data-acquisition time of 4 s was demonstrated. Five prepared gas mixtures and 15 exhaled breath samples were measured with both the NO sensor and for intercomparison with a chemiluminescence-based NO analyzer and were found to be in agreement within 0.6 ppbv. Exhaled NO flow-independent parameters, which may provide diagnostic and therapeutic information in respiratory diseases where single-breath measurements are equivocal, were estimated from end-tidal NO concentration measurements collected at various flow rates. The results of this work indicate that a laser-based exhaled NO sensor can be used to measure exhaled nitric oxide at a range of exhalation flow rates to determine flow-independent parameters in human clinical trials. PACS 07.07.Df; 33.20.Ea; 42.62.Fi; 87.80.-y     

Optical parametric oscillator based difference frequency laser source for photoacoustic trace gas spectroscopy in the 3 μm mid-IR range

We report on the extension of the emission wavelength range of a nanosecond pulsed commercial optical parametric oscillator (OPO) towards the infrared. By difference frequency mixing the idler of the OPO with the fundamental of its Nd:YAG pump laser the wavelength range from 2.5–4.5 μm is covered at considerable pulse energies. This laser source is then applied for the first time to photoacoustic trace gas spectroscopy in the fundamental C---H stretch band located around 3.3 μm. Spectra of single- and multi-component gas mixtures of volatile organic compounds are recorded and analyzed with respect to composition and concentration. The detection limits for the individual substances within the gas mixtures are found in the lower parts per million (ppm) range.     

Asynchronous midinfrared ultrafast optical parametric oscillator for dual-comb spectroscopy

Two asynchronous, broadband 3.3 μm pulse trains with a stabilized repetition-rate difference of up to 5 kHz were generated using an ultrafast optical parametric oscillator. The two oscillation channels, each producing ～100 mW average power, ran essentially independently, and weak non-phase-matched sum-frequency mixing between them provided a timing signal that indicated when the asynchronous pulses coincided. The system has immediate applications in incoherent asynchronous optical sampling and, with additional carrier-envelope-offset stabilization, could be applied to coherent dual-frequency-comb spectroscopy.     

A narrow-linewidth optical parametric oscillator for mid-infrared high-resolution spectroscopy

We present a narrow-linewidth, singly-resonant cw optical parametric oscillator, emitting more than 1 W in the 2.7–4.2?µm range. The OPO is pumped by a narrow linewidth (40?kHz) fibre-laser system and the signal frequency is locked to a high-finesse Fabry–Pérot cavity in order to increase the spectral resolution, thus obtaining a residual linewidth of 70?kHz for the signal. We tested the spectral performance of our OPO on several transitions in the ν₁ rovibrational band of CH₃I, measuring line intensities and showing sub-Doppler dip detection.     

Simultaneous 13C/12C and (18)O/(16)O isotope ratio measurements on CO2 based on off-axis integrated cavity output spectroscopy

A prototype off-axis integrated cavity output spectrometer (OA-ICOS) utilizing two identical cavities together with a near-infrared (1.63 microm) external cavity tunable diode laser is described. The two-cavity design-one for a reference gas and one for a sample gas-takes advantage of classical double-beam infrared spectrometer characteristics in reducing uncertainties due to laser scan or power instabilities and major temperature variations by a factor of three or better compared with a single-cavity scheme. This is the first OA-ICOS instrument designed to determine 13C/12C and (18)O/(16)O ratios from CO2 rotation/vibration fine structure in three different combination bands. Preliminary results indicate that at 0.8 Hz a precision of 3.3 and 2.8 per thousand is obtained for delta13C and delta(18)O, respectively, over a period of 10 h and a pure CO2 gas sample at 26 hPa. By averaging 100 spectra over a subset of the data, we achieved a precision of 1.6 and 0.8 \permil\ for delta13C and delta(18)O, respectively.     

Terahertz-wave parametric oscillator with a misalignment-resistant tuning cavity

We demonstrate a terahertz-wave parametric oscillator (TPO) with a corner-cube resonator consisting of a corner-cube prism (CCP) and a flat mirror. By using the cavity configuration proposed in this Letter, the generation of tunable monochromatic terahertz (THz) waves can be achieved just by rotating the flat mirror instead of rotating the TPO cavity relative to the pump beam. The THz-wave output intensity and pulse width can be controlled periodically by rotating the CCP around the cavity axis. The TPO stability against cavity misalignment is significantly improved by at least 1 to 2 orders of magnitude compared with the conventional plane-parallel resonator configuration.     

Continuous wave optical parametric oscillator for quartz-enhanced photoacoustic trace gas sensing

A continuous wave optical parametric oscillator, generating up to 300 mW idler output in the 3–4 μm wavelength region, and pumped by a fiber-amplified DBR diode laser is used for trace gas detection by means of quartz-enhanced photoacoustic spectroscopy (QEPAS). Mode-hop-free tuning of the OPO output over 5.2 cm^-1 and continuous spectral coverage exceeding 16.5 cm^-1 were achieved via electronic pump source tuning alone. Online monitoring of the idler wavelength, with feedback to the DBR diode laser, provided an automated closed-loop control allowing arbitrary idler wavelength selection within the pump tuning range and locking of the idler wavelength with a stability of 1.7×10^-3 cm^-1 over at least 30 min. Using this approach, we locked the idler wavelength at an ethane absorption peak and obtained QEPAS data to verify the linear response of the QEPAS signal at different ethane concentrations (100 ppbv-20 ppmv) and different power levels. The detection limit for ethane was determined to be 13 ppbv (20 s averaging), corresponding to a normalized noise equivalent absorption coefficient of 4.4×10^-7 cm^-1  W/Hz^1/2. PACS 42.55.Wd; 42.65.Yj; 42.62.Fi