1. |
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2. |
- Axner, Ove, 1957-, et al.
(author)
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NICE-OHMS – frequency modulation cavity-enhanced spectroscopy : principles and performance
- 2014
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In: Cavity-Enhanced Spectroscopy and Sensing. - Berlin : Springer Berlin/Heidelberg. - 9783642400025 - 9783642400032 ; , s. 221-251
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Book chapter (peer-reviewed)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is a sensitive technique for detection of molecular species in gas phase. It is based on a combination of frequency modulation for reduction of noise and cavity enhancement for prolongation of the interaction length between the light and a sample. It is capable of both Doppler-broadened and sub-Doppler detection with absorption sensitivity down to the 10−12 and 10−14 Hz−1/2 cm−1 range, respectively. This chapter provides a thorough description of the basic principles and the performance of the technique.
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3. |
- Ehlers, Patrick, 1981-, et al.
(author)
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Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry incorporating an optical circulator
- 2014
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In: Optics Letters. - : Optical Society of America. - 0146-9592 .- 1539-4794. ; 39:2, s. 279-282
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Journal article (peer-reviewed)abstract
- To reduce the complexity of fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry, a system incorporating a fiber-coupled optical circulator to deflect the cavity-reflected light for laser stabilization has been realized. Detection near the shot-noise limit has been demonstrated for both Doppler-broadened and sub-Doppler signals, yielding a lowest detectable absorption and optical phase shift of 2.2 x 10(-12) cm(-1) and 4.0 x 10(-12) cm(-1), respectively, both for a 10 s integration time, where the former corresponds to a detection limit of C2H2 of 5 ppt. (C) 2014 Optical Society of America
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4. |
- Ehlers, Patrick, 1981-, et al.
(author)
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Use of etalon-immune distances to reduce the influence of background signals in frequency-modulation spectroscopy and noise-immune cavity-enhanced optical heterodyne molecular spectroscopy
- 2014
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In: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 31:12, s. 2938-2945
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Journal article (peer-reviewed)abstract
- The detection sensitivity of phase-modulated techniques such as frequency-modulation spectroscopy (FMS) and noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is often limited by etalon background signals. It has previously been shown that the impact of etalons can be reduced by the use of etalon-immune distances (EIDs), i.e., by separating the surfaces that give rise to etalons by a distance of q. L-m, where L-m is given by c/2n nu(m), where, in turn, n and nu(m) are the index of refraction between the components that make up the etalon (thus most often that of air) and the modulation frequency, respectively, and where q is an integer (i.e., 1, 2, 3,.) or half-integer (i.e., 1/2, 1, 3/2,.) for the dispersion and absorption modes of detection, respectively. An etalon created by surfaces separated by an EID will evade detection and thereby not contribute to any background signal. The concept of EIDs in FMS and NICE-OHMS is in this work demonstrated, scrutinized, and discussed in some detail. It is shown that the influence of EIDs on the absorption and dispersion modes of detection is significantly different; signals detected at the dispersion phase are considerably less sensitive to deviations from exact EID conditions than those detected at the absorption phase. For example, the FM background signal from an etalon whose length deviates from an EID by 2.5% of L-m (e.g., by 1 cm for an L-m of 40 cm), detected in dispersion, is only 9% of that in absorption. This makes the former mode of detection the preferred one whenever a sturdy immunity against etalons is needed or when optical components with parallel surfaces (e.g., lenses, polarizers, or beam splitters) are used. The impact of the concept of EIDs on NICE-OHMS is demonstrated by the use of Allan-Werle plots.
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5. |
- Rutkowski, Lucile, et al.
(author)
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Experimental 1.5-1.6 μm water line list at 1950 K
- 2018
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In: Optics InfoBase Conference Papers. - : Optica Publishing Group. - 9781943580477
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Conference paper (peer-reviewed)abstract
- We demonstrate a high-temperature water absorption spectrum measured in a flame using cavity-enhanced frequency comb-based Fourier transform spectroscopy. The retrieved transition intensities and frequencies are assigned using the POKAZATEL line list.
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6. |
- Vieira, Francisco Senna, et al.
(author)
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Robust, Fast and Sensitive Near-Infrared Continuous-Filtering Vernier Spectrometer
- 2020
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In: 2020 Conference on Lasers and Electro-Optics (CLEO). - : IEEE. - 9781943580767 ; , s. 1-2
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Conference paper (peer-reviewed)abstract
- We present a new robust approach to cavity-enhanced comb spectroscopy based on Vernier filtering, a fixed diffraction grating, custom-made chopper wheel, and a low bandwidth comb-cavity stabilization scheme. We measure a CO2 spectrum with a few GHz resolution and 5 x 10-8 cm-1 sensitivity in 9.4 ms.
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7. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Broadband molecular detection with cavity-enhanced optical frequency comb spectroscopy
- 2014
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In: Optical instrumentation for energy and environmental applications, E2 2014. - Washington, D.C. : Optical Society of America (OSA). - 9781557527561
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Conference paper (peer-reviewed)abstract
- We demonstrate detection of atmospheric species in air and combustion environment using near-infrared cavity-enhanced optical frequency comb spectroscopy based on an Er:fiber femtosecond laser and a fast-scanning Fourier transform spectrometer.
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8. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Cavity-enhanced optical frequency comb spectroscopy in the mid-infrared application to trace detection of hydrogen peroxide
- 2013
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In: Applied physics. B, Lasers and optics (Print). - : Springer. - 0946-2171 .- 1432-0649. ; 110:2, s. 163-175
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Journal article (peer-reviewed)abstract
- We demonstrate the first cavity-enhanced optical frequency comb spectroscopy in the mid-infrared wavelength region and report the sensitive real-time trace detection of hydrogen peroxide in the presence of a large amount of water. The experimental apparatus is based on a mid-infrared optical parametric oscillator synchronously pumped by a high-power Yb:fiber laser, a high-finesse broadband cavity, and a fast-scanning Fourier transform spectrometer with autobalancing detection. The comb spectrum with a bandwidth of 200 nm centered around 3.76 μm is simultaneously coupled to the cavity and both degrees of freedom of the comb, i.e. the repetition rate and carrier envelope offset frequency, are locked to the cavity to ensure stable transmission. The autobalancing detection scheme reduces the intensity noise by a factor of 300, and a sensitivity of 5.4×10-9 cm-1 Hz-1/2 with a resolution of 800 MHz is achieved (corresponding to 6.9×10-11 cm-1 Hz-1/2 per spectral element for 6000 resolved elements). This yields a noise equivalent detection limit for hydrogen peroxide of 8 parts-per-billion (ppb); in the presence of 2.8 % of water the detection limit is 130 ppb. Spectra of acetylene, methane, and nitrous oxide at atmospheric pressure are also presented, and a line-shape model is developed to simulate the experimental data.
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9. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Cavity-enhanced optical frequency combs spectroscopy in the near- and mid-infrared
- 2016
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In: Imaging and applied optics 2016. - : OSA - The Optical Society. - 9781943580156
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Conference paper (peer-reviewed)abstract
- We present the recent developments in high-resolution Fourier transform spectroscopy based on optical frequency combs for precision measurements and combustion diagnostics, and the first implementation of continuous-filtering Vernier spectroscopy in the mid-infrared wavelength range for fast multispecies detection.
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10. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Characterization of fiber-laser-based sub-Doppler NICE-OHMS for quantitative trace gas detection
- 2008
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In: Optics Express. - 1094-4087. ; 16:19, s. 14689-14702
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Journal article (peer-reviewed)abstract
- The potential of fiber-laser-based sub-Doppler noise-immune cavity-enhanced optical heterodyne molecular spectrometry for trace gas detection is scrutinized. The non-linear dependence of the on-resonance sub-Doppler dispersion signal on the intracavity pressure and power is investigated and the optimum conditions with respect to these are determined. The linearity of the signal strength with concentration is demonstrated and the dynamic range of the technique is discussed. Measurements were performed on C2H2 at 1531 nm up to degrees of saturation of 100. The minimum detectable sub-Doppler optical phase shift was 5 x 10-11 cm-1 Hz-1/2, corresponding to a partial pressure of C2H2 of 1 x 10-12 atm for an intracavity pressure of 20 mTorr, and a concentration of 10 ppb at 400 mTorr.
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11. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry signals from optically saturated transitions under low pressure conditions
- 2008
-
In: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 25:7, s. 1156-1165
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Journal article (peer-reviewed)abstract
- The influence of optical saturation on noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) signals from purely Doppler-broadened transitions is investigated experimentally. It is shown that the shape and the strength of the dispersion signal are virtually unaffected by optical saturation, whereas the strength of the absorption signal decreases as (1+G+-1)-1/2, where G+-1 is the degree of saturation induced by the sideband of the frequency modulated triplet, in agreement with theoretical predictions. This implies, first of all, that Doppler-broadened NICE-OHMS is affected less by optical saturation than other cavity enhanced techniques but also that it exhibits nonlinearities in the power and pressure dependence for all detection phases except pure dispersion. A methodology for assessments of the degree of saturation and the saturation power of a transition from Doppler-broadened NICE-OHMS signals is given. The implications of optical saturation for practical trace species detection by Doppler-broadened NICE-OHMS are discussed.
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12. |
- Foltynowicz, Aleksandra, 1981-
(author)
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Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry
- 2009
-
Doctoral thesis (other academic/artistic)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectro-metry (NICE-OHMS) is one of the most sensitive laser-based absorption techniques. The high sensitivity of NICE-OHMS is obtained by a unique combination of cavity enhancement (for increased interaction length with a sample) with frequency modulation spectrometry (for reduction of noise). Moreover, sub-Doppler detection is possible due to the presence of high intensity counter-propagating waves inside an external resonator, which provides an excellent spectral selectivity. The high sensitivity and selectivity make NICE-OHMS particularly suitable for trace gas detection. Despite this, the technique has so far not been often used for practical applications due to its technical complexity, originating primarily from the requirement of an active stabilization of the laser frequency to a cavity mode.The main aim of the work presented in this thesis has been to develop a simpler and more robust NICE-OHMS instrumentation without compro-mising the high sensitivity and selectivity of the technique. A compact NICE-OHMS setup based on a fiber laser and a fiber-coupled electro-optic modulator has been constructed. The main advantage of the fiber laser is its narrow free-running linewidth, which significantly simplifies the frequency stabilization procedure. It has been demonstrated, using acetylene and carbon dioxide as pilot species, that the system is capable of detecting relative absorption down to 3 × 10-9 on a Doppler-broadened transition, and sub-Doppler optical phase shift down to 1.6 × 10-10, the latter corresponding to a detection limit of 1 × 10-12 atm of C2H2. Moreover, the potential of dual frequency modulation dispersion spectrometry (DFM-DS), an integral part of NICE-OHMS, for concentration measurements has been assessed.This thesis contributes also to the theoretical description of Doppler-broadened and sub-Doppler NICE-OHMS signals, as well as DFM-DS signals. It has been shown that the concentration of an analyte can be deduced from a Doppler-broadened NICE-OHMS signal detected at an arbitrary and unknown detection phase, provided that a fit of the theoretical lineshape to the experimental data is performed. The influence of optical saturation on Doppler-broadened NICE-OHMS signals has been described theoretically and demonstrated experimentally. In particular, it has been shown that the Doppler-broadened dispersion signal is unaffected by optical saturation in the Doppler limit. An expression for the sub-Doppler optical phase shift, valid for high degrees of saturation, has been derived and verified experimentally up to degrees of saturation of 100.
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13. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Measurement and assignment of double-resonance transitions to the 8900-9100- cm-1 levels of methane
- 2021
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In: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 103:2
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Journal article (peer-reviewed)abstract
- Optical-optical double-resonance spectroscopy with a continuous wave pump and frequency comb probe allows measurement of sub-Doppler transitions to highly excited molecular states over a wide spectral range with high frequency accuracy. We report on assessment and characterization of sub-Doppler double-resonance transitions in methane measured using a 3.3-μm continuous wave optical parametric oscillator as a pump and a 1.67-μm frequency comb as a probe. The comb spectra were recorded using a Fourier transform spectrometer with comb-mode-limited resolution. With the pump tuned to nine different transitions in the ν3 fundamental band, we detected 36 ladder-type transitions to the 3ν3 overtone band region, and 18 V-type transitions to the 2ν3 overtone band. We describe in detail the experimental approach and the pump stabilization scheme, which currently limits the frequency accuracy of the measurement. We present the data analysis procedure used to extract the frequencies and intensities of the probe transitions for parallel and perpendicular relative pump-probe polarization. We compare the center frequencies and relative intensities of the ladder-type transitions to theoretical predictions from the TheoReTS and ExoMol line lists, demonstrating good agreement with TheoReTS.
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14. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Noise-immune cavity-enhanced optical heterodyne molecular spectrometry : Current status and future potential
- 2008
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In: Applied physics. B, Lasers and optics (Print). - Berlin / Heidelberg : Springer Berlin/Heidelberg. - 0946-2171 .- 1432-0649. ; 92:3, s. 313-326
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Journal article (peer-reviewed)abstract
- As a result of a combination of an external cavity and modulation techniques, noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is one of the most sensitive absorption techniques, capable of reaching close-to-shot-noise sensitivities, down to 5×10-13 fractional absorption at 1 s averaging. Due to its ability to provide sub-Doppler signals from weak molecular overtone transitions, the technique was first developed for frequency standard applications. It has since then also found use in fields of molecular spectroscopy of weak overtone transitions and trace gas detection. This paper describes the principles and the unique properties of NICE-OHMS. The historical background, the contributions of various groups, as well as the performance and present status of the technique are reviewed. Recent progress is highlighted and the future potential of the technique for trace species detection is discussed.
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15. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Sub-Doppler Double-Resonance Spectroscopy of Methane Using a Frequency Comb Probe
- 2021
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In: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 126:6
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Journal article (peer-reviewed)abstract
- We report the first measurement of sub-Doppler molecular response using a frequency comb by employing the comb as a probe in optical-optical double-resonance spectroscopy. We use a 3.3 μm continuous wave pump and a 1.67 μm comb probe to detect sub-Doppler transitions to the 2ν3 and 3ν3 bands of methane with ∼1.7 MHz center frequency accuracy. These measurements provide the first verification of the accuracy of theoretical predictions from highly vibrationally excited states, needed to model the high-temperature spectra of exoplanets. Transition frequencies to the 3ν3 band show good agreement with the TheoReTS line list.
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16. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Sub-doppler double-resonance spectroscopy of methane using a frequency comb probe
- 2020
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In: Conference on Lasers and Electro-Optics. - : Optica Publishing Group (formerly OSA). - 9781943580767 - 9781728144184
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Conference paper (peer-reviewed)abstract
- We use a 3.3 µm continuous wave optical parametric oscillator as a pump and a 1.67 µm frequency comb as a probe to record 36 sub-Doppler double-resonance transitions in the 3v3 band of methane (including 26 previously unreported) with ~1.5 MHz center frequency accuracy.
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17. |
- Foltynowicz, Aleksandra, 1981-, et al.
(author)
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Wavelength modulated noise-immune cavity-enhanced optical heterodyne molecular spectroscopy signal line shapes in the Doppler limit
- 2009
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In: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 26:7, s. 1384-1394
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Journal article (peer-reviewed)abstract
- A thorough analysis of the shape and strength of Doppler-broadened wavelength modulated noise-immune cavity-enhanced optical heterodyne molecular spectroscopy signals is presented and their dependence on modulation frequency, modulation amplitude and detection phase is investigated in detail. The conditions that maximize the on-resonance signal are identified. The analysis is based on the standard frequency modulation spectroscopy formalism and the Fourier description of wavelength modulation spectroscopy and verified by fits to experimental signals from C2H2 and CO2 measured at 1531 nm. In addition, the line strengths of two CO2 transitions in the v2→3v1+v2+v3 hot band [Pe(7) and Pe(9)] were found to differ by ~20% from those given in the HITRAN database.
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18. |
- Foltynowicz-Matyba, Aleksandra, 1981-, et al.
(author)
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Reduction of background signals in fiber-based NICE-OHMS
- 2011
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In: Journal of the Optical Society of America. B, Optical physics. - Washington, D.C. : Optical Society of America. - 0740-3224 .- 1520-8540. ; 28:11, s. 2797-2805
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Journal article (peer-reviewed)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) based on a fiber-coupled electro-optic modulator (EOM) provides a compact and versatile experimental setup. It has, however, been limited by background signals originating from an imbalance of the phase modulated triplet created by a cross-coupling between the principal axes of the polarization maintaining fibers and the extraordinary axis of the EOM. Two strategies for reducing these background signals are investigated: (i) using an EOM with a titanium diffused waveguide, in which the balance of the triplet is controlled by active feedback, and (ii) using an EOM with a proton exchanged waveguide that does not support light propagation along the ordinary axis. It is shown that both approaches significantly reduce drifts and noise in the system. Using a cavity with a finesse of 5700, an absorption sensitivity of 3: 2 x 10(-12) cm(-1) in 1 min of integration time (i.e., 1: 8 x 10(-11) cm(-1) Hz(-1/2)) is demonstrated for Doppler-broadened detection, the lowest reported so far for Doppler-broadened NICE-OHMS. For sub-Doppler detection, a minimum detectable optical phase shift of 1: 3 x 10(-12) cm(-1) in 400s of integration time is obtained. (C) 2011 Optical Society of America
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19. |
- Germann, Matthias, et al.
(author)
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A methane line list with sub-MHz accuracy in the 1250 to 1380 cm−1 range from optical frequency comb Fourier transform spectroscopy
- 2022
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In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier BV. - 0022-4073 .- 1879-1352. ; 288
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Journal article (peer-reviewed)abstract
- We use a Fourier transform spectrometer based on a difference frequency generation optical frequency comb to measure high-resolution, low-pressure, room-temperature spectra of methane in the 1250 – 1380-cm−1 range. From these spectra, we retrieve line positions and intensities of 678 lines of two isotopologues: 157 lines from the 12CH4 ν4 fundamental band, 131 lines from the 13CH4 ν4 fundamental band, as well as 390 lines from two 12CH4 hot bands, ν2 + ν4 – ν2 and 2ν4 – ν4. For another 165 lines from the 12CH4 ν4 fundamental band we retrieve line positions only. The uncertainties of the line positions range from 0.19 to 2.3 MHz, and their median value is reduced by a factor of 18 and 59 compared to the previously available data for the 12CH4 fundamental and hot bands, respectively, obtained from conventional FTIR absorption measurements. The new line positions are included in the global models of the spectrum of both methane isotopologues, and the fit residuals are reduced by a factor of 8 compared to previous absorption data, and 20 compared to emission data. The experimental line intensities have relative uncertainties in the range of 1.5 – 7.7%, similar to those in the previously available data; 235 new 12CH4 line intensities are included in the global model.
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20. |
- Germann, Matthias, et al.
(author)
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An Accurate Methane Line List in the 7.2-8.0 µm Range from Comb-Based Fourier Transform Spectroscopy
- 2022
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In: CLEO: 2022. - : Optica Publishing Group. - 9781557528209
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Conference paper (peer-reviewed)abstract
- We use comb-based Fourier transform spectroscopy to record high-resolution spectra of 12CH4 and 13CH4 from 1250 to 1380 cm-1. We obtain line positions and intensities of 4 bands with uncertainties of ~450 kHz and ~3%, respectively, which we use to improve a global fit of the effective Hamiltonian.
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22. |
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23. |
- Germann, Matthias, et al.
(author)
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Optical frequency comb Fourier transform spectroscopy of formaldehyde in the 1250 to 1390 cm−1 range : experimental line list and improved MARVEL analysis
- 2024
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In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier. - 0022-4073 .- 1879-1352. ; 312
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Journal article (peer-reviewed)abstract
- We use optical frequency comb Fourier transform spectroscopy to record high-resolution, low-pressure, room-temperature spectra of formaldehyde (H212C16O) in the range of 1250 to 1390 cm−1. Through line-by-line fitting, we retrieve line positions and intensities of 747 rovibrational transitions: 558 from the ν6 band, 129 from the ν4 band, and 14 from the ν3 band, as well as 46 from four different hot bands. We incorporate the accurate and precise line positions (0.4 MHz median uncertainty) into the MARVEL (measured active vibration-rotation energy levels) analysis of the H2CO spectrum. This increases the number of MARVEL-predicted energy levels by 82 and of rovibrational transitions by 5382, and substantially reduces uncertainties of MARVEL-derived H2CO energy levels over a large range: from pure rotational levels below 200 cm−1 up to multiply excited vibrational levels at 6000 cm−1. This work is an important step toward filling the gaps in formaldehyde data in the HITRAN database.
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24. |
- Germann, Matthias, et al.
(author)
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Precision frequency comb spectroscopy in the 8 µm range
- 2023
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In: CLEO 2023. - : Optical Society of America. - 9781957171258
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Conference paper (peer-reviewed)abstract
- We use Fourier transform spectroscopy based on a compact difference frequency generation comb source emitting around 8 μm to record broadband high-resolution spectra of molecules relevant to astrophysics and environmental monitoring. From the spectra we obtain line lists with sub-MHz accuracy, an order of magnitude better than previously available, and use them to refine theoretical models of these molecules. Here we report results for formaldehyde, for which the 8 μm range is missing in HITRAN.
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25. |
- Gluszek, Aleksander, et al.
(author)
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Compact mode-locked Er-doped fiber laser for broadband cavity-enhanced spectroscopy
- 2020
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In: Applied physics. B, Lasers and optics (Print). - : Springer. - 0946-2171 .- 1432-0649. ; 126:8
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Journal article (peer-reviewed)abstract
- We report the design and characteristics of a simple and compact mode-locked Er-doped fiber laser and its application to broadband cavity-enhanced spectroscopy. The graphene mode-locked polarization maintaining oscillator consumes less than 5 W of power. It is thermally stabilized, enclosed in a 3D printed box, and equipped with three actuators that control the repetition rate: fast and slow fiber stretchers, and metal-coated fiber section. This allows wide tuning of the repetition rate and its stabilization to an external reference source. The applicability of the laser to molecular spectroscopy is demonstrated by detecting CO(2)in air using continuous-filtering Vernier spectroscopy with absorption sensitivity of 5.5 x 10(-8)cm(-1)in 50 ms.
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