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1.
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2.
  • Axner, Ove, 1957-, et al. (author)
  • NICE-OHMS – frequency modulation cavity-enhanced spectroscopy : principles and performance
  • 2014
  • In: Cavity-Enhanced Spectroscopy and Sensing. - Berlin : Springer Berlin/Heidelberg. - 9783642400025 - 9783642400032 ; , s. 221-251
  • 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)
  • Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry incorporating an optical circulator
  • 2014
  • In: Optics Letters. - : Optical Society of America. - 0146-9592 .- 1539-4794. ; 39:2, s. 279-282
  • 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)
  • 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
  • In: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 31:12, s. 2938-2945
  • 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)
  • Experimental 1.5-1.6 μm water line list at 1950 K
  • 2018
  • In: Optics InfoBase Conference Papers. - : Optica Publishing Group. - 9781943580477
  • 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)
  • Robust, Fast and Sensitive Near-Infrared Continuous-Filtering Vernier Spectrometer
  • 2020
  • In: 2020 Conference on Lasers and Electro-Optics (CLEO). - : IEEE. - 9781943580767 ; , s. 1-2
  • 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)
  • Broadband molecular detection with cavity-enhanced optical frequency comb spectroscopy
  • 2014
  • In: Optical instrumentation for energy and environmental applications, E2 2014. - Washington, D.C. : Optical Society of America (OSA). - 9781557527561
  • 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)
  • Cavity-enhanced optical frequency comb spectroscopy in the mid-infrared application to trace detection of hydrogen peroxide
  • 2013
  • In: Applied physics. B, Lasers and optics (Print). - : Springer. - 0946-2171 .- 1432-0649. ; 110:2, s. 163-175
  • 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)
  • Cavity-enhanced optical frequency combs spectroscopy in the near- and mid-infrared
  • 2016
  • In: Imaging and applied optics 2016. - : OSA - The Optical Society. - 9781943580156
  • 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)
  • Characterization of fiber-laser-based sub-Doppler NICE-OHMS for quantitative trace gas detection
  • 2008
  • In: Optics Express. - 1094-4087. ; 16:19, s. 14689-14702
  • 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)
  • 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
  • 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)
  • 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)
  • Measurement and assignment of double-resonance transitions to the 8900-9100- cm-1 levels of methane
  • 2021
  • In: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 103:2
  • 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)
  • Noise-immune cavity-enhanced optical heterodyne molecular spectrometry : Current status and future potential
  • 2008
  • In: Applied physics. B, Lasers and optics (Print). - Berlin / Heidelberg : Springer Berlin/Heidelberg. - 0946-2171 .- 1432-0649. ; 92:3, s. 313-326
  • 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)
  • Sub-Doppler Double-Resonance Spectroscopy of Methane Using a Frequency Comb Probe
  • 2021
  • In: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 126:6
  • 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)
  • Sub-doppler double-resonance spectroscopy of methane using a frequency comb probe
  • 2020
  • In: Conference on Lasers and Electro-Optics. - : Optica Publishing Group (formerly OSA). - 9781943580767 - 9781728144184
  • 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)
  • Wavelength modulated noise-immune cavity-enhanced optical heterodyne molecular spectroscopy signal line shapes in the Doppler limit
  • 2009
  • In: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 26:7, s. 1384-1394
  • 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)
  • Reduction of background signals in fiber-based NICE-OHMS
  • 2011
  • 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
  • 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)
  • A methane line list with sub-MHz accuracy in the 1250 to 1380 cm−1 range from optical frequency comb Fourier transform spectroscopy
  • 2022
  • In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier BV. - 0022-4073 .- 1879-1352. ; 288
  • 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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22.
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23.
  • Germann, Matthias, et al. (author)
  • Optical frequency comb Fourier transform spectroscopy of formaldehyde in the 1250 to 1390 cm−1 range : experimental line list and improved MARVEL analysis
  • 2024
  • In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier. - 0022-4073 .- 1879-1352. ; 312
  • 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)
  • Precision frequency comb spectroscopy in the 8 µm range
  • 2023
  • In: CLEO 2023. - : Optical Society of America. - 9781957171258
  • 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)
  • Compact mode-locked Er-doped fiber laser for broadband cavity-enhanced spectroscopy
  • 2020
  • In: Applied physics. B, Lasers and optics (Print). - : Springer. - 0946-2171 .- 1432-0649. ; 126:8
  • 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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26.
  • Gordon, I.E., et al. (author)
  • The HITRAN2020 molecular spectroscopic database
  • 2022
  • In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier. - 0022-4073 .- 1879-1352. ; 277
  • Journal article (peer-reviewed)abstract
    • The HITRAN database is a compilation of molecular spectroscopic parameters. It was established in the early 1970s and is used by various computer codes to predict and simulate the transmission and emission of light in gaseous media (with an emphasis on terrestrial and planetary atmospheres). The HITRAN compilation is composed of five major components: the line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, experimental infrared absorption cross-sections (for molecules where it is not yet feasible for representation in a line-by-line form), collision-induced absorption data, aerosol indices of refraction, and general tables (including partition sums) that apply globally to the data. This paper describes the contents of the 2020 quadrennial edition of HITRAN. The HITRAN2020 edition takes advantage of recent experimental and theoretical data that were meticulously validated, in particular, against laboratory and atmospheric spectra. The new edition replaces the previous HITRAN edition of 2016 (including its updates during the intervening years). All five components of HITRAN have undergone major updates. In particular, the extent of the updates in the HITRAN2020 edition range from updating a few lines of specific molecules to complete replacements of the lists, and also the introduction of additional isotopologues and new (to HITRAN) molecules: SO, CH3F, GeH4, CS2, CH3I and NF3. Many new vibrational bands were added, extending the spectral coverage and completeness of the line lists. Also, the accuracy of the parameters for major atmospheric absorbers has been increased substantially, often featuring sub-percent uncertainties. Broadening parameters associated with the ambient pressure of water vapor were introduced to HITRAN for the first time and are now available for several molecules. The HITRAN2020 edition continues to take advantage of the relational structure and efficient interface available at www.hitran.org and the HITRAN Application Programming Interface (HAPI). The functionality of both tools has been extended for the new edition.
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28.
  • Hjältén, Adrian, 1988-, et al. (author)
  • Accurate measurement and assignment of high rotational energy levels of the 3v3 ← v3 band of methane
  • 2023
  • In: 2023 conference on lasers and electro-optics, CLEO 2023. - : IEEE. - 9781957171258 - 9781665455688
  • Conference paper (peer-reviewed)abstract
    • We use optical-optical double-resonance spectroscopy with a high-power continuous wave pump and a cavity-enhanced comb probe to expand sub-Doppler measurements of the 3v3 ← v3 band of CH4 to higher rotational levels. We assign the final states using combination differences, i.e., by reaching the same state using different pump/probe combinations.
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29.
  • Hjältén, Adrian, et al. (author)
  • Fourier transform spectroscopy using difference frequency generation comb sources at 3.3 µm and 7.8 µm
  • 2021
  • In: Proceedings OSA Optical Sensors and Sensing Congress 2021 (AIS, FTS, HISE, SENSORS, ES). - : Optical Society of America. - 9781557528209
  • Conference paper (peer-reviewed)abstract
    • We use offset-frequency-free difference frequency generation comb sources and a Fourier transform spectrometer with comb-mode-width limited resolution to measure and analyze spectra of molecular species of atmospheric relevance: CH3I and CH2Br2 around 3000 cm-1, and 14N216O around 1280 cm-1
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30.
  • Hjältén, Adrian, et al. (author)
  • High-Resolution Measurements of Halogenated Volatile Organic Compounds Using Frequency Comb Fourier Transform Spectroscopy
  • 2021
  • In: 2021 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2021. - : IEEE Lasers and Electro-Optics Society. - 9781665418768
  • Conference paper (peer-reviewed)abstract
    • Halogenated volatile organic compounds (HVOCs) play an important role in the photo-chemistry of the atmosphere, for example in ozone depletion [1]. They are produced naturally in the oceans but are also used in industrial and agricultural applications where they may pose a health-hazard due to their biological effects. Optical detection of these compounds would hence be of great value in, for example, atmospheric monitoring and leak detection in workplaces. Crucial for such detection schemes is access to accurate spectroscopic models, which in turn require high-precision laboratory measurements. Due to the combination of broad spectral coverage and high resolution, optical frequency comb Fourier transform spectroscopy is an excellent tool for providing the necessary spectroscopic data. We use a mid-infrared frequency comb and a Fourier transform spectrometer (FTS) to measure and assign high-resolution spectra of multiple absorption bands of two HVOCs: methyl iodide, CH 3 I [2] , and dibromomethane, CH 2 Br 2 , around 3.3m.
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31.
  • Hjältén, Adrian, et al. (author)
  • Line positions and intensities of the ν1 band of 12CH3I using mid-infrared optical frequency comb Fourier transform spectroscopy
  • 2023
  • In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier. - 0022-4073 .- 1879-1352. ; 306
  • Journal article (peer-reviewed)abstract
    • We present a new spectral analysis of the ν1 and ν3+ν1−ν3 bands of 12CH3I around 2971 cm−1 based on a high-resolution spectrum spanning from 2800 cm–1 to 3160 cm–1, measured using an optical frequency comb Fourier transform spectrometer. From this spectrum, we previously assigned the ν4 and ν3+ν4−ν3 bands around 3060 cm–1 using PGOPHER, and the line list was incorporated in the HITRAN database. Here, we treat the two fundamental bands, ν1 and ν4, together with the perturbing states, 2ν2+ν3 and ν2+2ν6±2, as a four-level system connected via Coriolis and Fermi interactions. A similar four-level system is assumed to connect the two ν3+ν1−ν3 and ν3+ν4−ν3 hot bands, which appear due to the population of the low-lying ν3 state at room temperature, with the 2ν2+2ν3 and ν2+ν3+2ν6±2 perturbing states. This spectroscopic treatment provides a good global agreement of the simulated spectra with experiment, and hence accurate line lists and band parameters of the four connected vibrational states in each system. It also allows revisiting the analysis of the ν4 and ν3+ν4−ν3 bands, which were previously treated as separate bands, not connected to their ν1 and ν3+ν1−ν3 counterparts. Overall, we assign 4665 transitions in the fundamental band system, with an average error of 0.00071 cm–1, a factor of two better than earlier work on the ν1 band using conventional Fourier transform infrared spectroscopy. The ν1 band shows hyperfine splitting, resolvable for transitions with J ≤ 2 × K. Finally, the spectral intensities of 65 lines of the ν1 band and 7 lines of the ν3+ν1−ν3 band are reported for the first time using the Voigt line shape as a model in multispectral fitting. The reported line lists and intensities will serve as a reference for high-resolution molecular spectroscopic databases, and as a basis for line selection in future monitoring applications of CH3I.
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32.
  • Hjältén, Adrian, et al. (author)
  • Optical frequency comb Fourier transform spectroscopy of 14N216O at 7.8 µm
  • 2021
  • In: Journal of Quantitative Spectroscopy and Radiative Transfer. - : Elsevier. - 0022-4073 .- 1879-1352. ; 271
  • Journal article (peer-reviewed)abstract
    • We use a Fourier transform spectrometer based on a compact mid-infrared difference frequency generation comb source to perform broadband high-resolution measurements of nitrous oxide, 14N216O, and retrieve line center frequencies of the ν1 fundamental band and the ν1 + ν2 – ν2 hot band. The spectrum spans 90 cm−1 around 1285 cm−1 with a sample point spacing of 3 × 10−4 cm−1 (9 MHz). We report line positions of 72 lines in the ν1 fundamental band between P(37) and R(38), and 112 lines in the ν1 + ν2 – ν2 hot band (split into two components with e/f rotationless parity) between P(34) and R(33), with uncertainties in the range of 90-600 kHz. We derive upper state constants of both bands from a fit of the effective ro-vibrational Hamiltonian to the line center positions. For the fundamental band, we observe excellent agreement in the retrieved line positions and upper state constants with those reported in a recent study by AlSaif et al. using a comb-referenced quantum cascade laser [J Quant Spectrosc Radiat Transf, 2018;211:172-178]. We determine the origin of the hot band with precision one order of magnitude better than previous work based on FTIR measurements by Toth [http://mark4sun.jpl.nasa.gov/n2o.html], which is the source of the HITRAN2016 data for these bands.
  •  
33.
  • Hjältén, Adrian, et al. (author)
  • Precision measurements of 14N216O using a comb-based fourier transform spectrometer at 7.8 µm
  • 2021
  • In: CLEO: Science and Innovations. - : Optical Society of America. - 9781557528209
  • Conference paper (peer-reviewed)abstract
    • Using a compact fiber-based difference frequency generation comb and a Fourier transform spectrometer we record spectra of the N2O ν1 band at 1285 cm-1 in the Doppler limit. Fitting Gaussian line shapes to the individual absorption lines yields center frequencies with <200 kHz average precision.
  •  
34.
  • Hjältén, Adrian, 1988- (author)
  • Precision molecular spectroscopy in the near- and mid-infrared using frequency comb-based Fourier transform spectrometers
  • 2023
  • Doctoral thesis (other academic/artistic)abstract
    • Absorption spectroscopy is a powerful scientific tool for non-invasive and remote sensing applications ranging from atmospheric monitoring to astrophysics. In spectroscopic detection schemes it is necessary to have spectral models for any molecular species to be detected or quantified. Such models are often based on spectroscopic measurements or at the very least require experimental validation. The experimental data need to be accurate in terms of absorption line positions and intensities, but should also cover as many absorption lines as possible, i.e. broadband measurements are highly desirable.Fourier transform spectroscopy (FTS) based on optical frequency combs (OFCs) can supply laboratory data that meet these requirements. OFCs provide a broad optical bandwidth and high spectral brightness, and also revolutionized our ability to measure optical frequencies, which had a profound impact on the frequency accuracy of spectroscopic measurements. The combination of OFCs and FTS, using the recently developed sub-nominal resolution technique, allows for measuring broadband absorption spectra with very high resolution, and a frequency accuracy provided by the OFCs. The aim of the work in this thesis was to expand the application of sub-nominal OFC-FTS to provide the much needed high-accuracy data for validation and development of spectroscopic databases of molecules relevant for a wide range of sensing application.We developed a spectrometer to target the strong molecular absorption bands in the mid-infrared using two OFC sources based on difference frequency generation (DFG) emitting in the 3 μm and 8 μm wavelength ranges. We measured the spectra of iodomethane, CH3I, and dibromomethane, CH2Br2, around 3 μm, fitted Hamiltonian models to several bands using the PGOPHER software, and reported molecular constants. For CH3I we improved on previous models, while for CH2Br2 we presented a new interpretation of the spectrum. We also reported the first assessments of line intensities of CH3I performed using multispectral fitting. At 8 μm, we implemented OFC-FTS based on a fiber-based compact DFG OFC source and measured low pressure spectra of nitrous oxide, N2O, methane, CH4, and formaldehyde, H2CO. After the frequency accuracy was confirmed by excellent agreement with an earlier accurate study of N2O, we compiled extensive line lists for CH4 and H2CO containing hundreds of transition frequencies with a precision improved by one order of magnitude compared to previously available data, and also reported line intensities for most transitions. For CH4 the new data were used to improve a global Hamiltonian model, while the H2CO data were incorporated into an algorithm based on spectroscopic networks to yield better precision in predicted energy levels and transition frequencies.We also further developed a recent implementation of double resonance (DR) spectroscopy where optical pumping by a continuous-wave laser was used to populate selected vibrational energy levels of CH4 not populated at room temperature, and a near-infrared OFC probed sub-Doppler transitions from the pumped states. Such measurements are necessary to validate theoretical predictions of transitions between excited vibrational levels that are relevant for high-temperature environments such as the atmospheres of hot celestial objects. We reported an improved measurement setup using a new pump laser, new enhancement cavity with an updated OFC-cavity locking scheme, and measured transitions between more highly excited rotational levels than was previously reported. The higher rotational excitations lead to a larger number of DR transitions, which could be readily detected in the broadband high-resolution OFC-FTS spectra. We retrieved parameters of 88 lines of which we could assign 79 to theoretically predicted transitions. We found systematic frequency discrepancies with the predictions, that had not been observed earlier for lower rotational levels.These implementations of sub-nominal OFC-FTS thus provided highly accurate line lists and improved spectral models of absorption bands of several molecules in the universally important mid-infrared region, as well as the first detection of 88 transitions between excited vibrational states of CH4 relevant for high-temperature environments. We demonstrated the high potential of these techniques for collecting large amounts of accurate spectroscopic data, that further the scope of applicability of molecular spectroscopy.
  •  
35.
  • Johansson, Alexandra C., et al. (author)
  • Broadband calibration-free cavity-enhanced complex refractive index spectroscopy using a frequency comb
  • 2018
  • In: Optics Express. - : Optical Society of America. - 1094-4087. ; 26:16, s. 20633-20648
  • Journal article (peer-reviewed)abstract
    • We present broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), a technique for calibration-free determination of the complex refractive index of entire molecular bands via direct measurement of transmission modes of a Fabry-Perot cavity filled with the sample. The measurement of the cavity transmission spectrum is done using an optical frequency comb and a mechanical Fourier transform spectrometer with sub-nominal resolution. Molecular absorption and dispersion spectra (corresponding to the imaginary and real parts of the refractive index) are obtained from the cavity mode broadening and shift retrieved from fits of Lorentzian profiles to the individual cavity modes. This method is calibration-free because the mode broadening and shift are independent of the cavity parameters such as the length and mirror reflectivity. In this first demonstration of broadband CE-CRIS we measure simultaneously the absorption and dispersion spectra of three combination bands of CO2 in the range between 1525 nm and 1620 nm and achieve good agreement with theoretical models. This opens up for precision spectroscopy of the complex refractive index of several molecular bands simultaneously. 
  •  
36.
  • Johansson, Alexandra C., 1987-, et al. (author)
  • Broadband Complex Refractive Index Spectroscopy via Measurement of Cavity Modes
  • 2018
  • In: 2018 Conference on Lasers and Electro-Optics (CLEO). - : IEEE. - 9781943580422
  • Conference paper (peer-reviewed)abstract
    • We retrieve high precision absorption and dispersion spectra of the 3v(1)+v(3) band of CO2 from direct measurement of cavity transmission modes using an optical frequency comb and a mechanical Fourier transfolin spectrometer with sub-nominal resolution.
  •  
37.
  •  
38.
  •  
39.
  • Johansson, Alexandra C., et al. (author)
  • Faraday rotation spectroscopy using an optical frequency comb
  • 2017
  • In: 2017 Conference on Lasers and Electro-Optics Europe &amp; European Quantum Electronics Conference (CLEO/Europe-EQEC). - : IEEE. - 9781509067367
  • Conference paper (peer-reviewed)abstract
    • Summary form only given. The mid-infrared (MIR) part of the optical spectrum (3-12 μm) houses the fundamental absorption bands of a multitude of environmentally important molecules, but the abundance of water absorption often causes interference with the target species and makes concentration measurement inaccurate. The broad spectral coverage of optical frequency comb spectroscopy (OFCS) provides access to entire ro-vibrational bands and allows more accurate concentration quantification and retrieval of sample temperature. To further improve detection sensitivity of paramagnetic species in the presence of interfering species, we combine a MIR optical frequency comb with the Faraday rotation spectroscopy (FRS) technique [I], which is insensitive to interferences from diamagnetic molecules, such as H 2 O, CO 2 , and CO. In FRS, the rotation of the polarization induced by an external magnetic field in the vicinity of paramagnetic molecular transitions is translated to an intensity change by the use of a polarization analyzer, which effectively removes the influence of any non-paramagnetic species. In the proof of principle demonstration of OFC-FRS we detect nitric oxide (NO) in the presence of water at 5.3 μm using a Fourier transform spectrometer.
  •  
40.
  • Johansson, Alexandra C., 1987-, et al. (author)
  • Fourier-transform-based noise-immune cavity-enhanced optical frequency comb spectroscopy
  • 2016
  • In: Light, Energy and the Environment. - : Optica Publishing Group (formerly OSA). - 9781557528209
  • Conference paper (peer-reviewed)abstract
    • We describe the principles and implementation of Fourier-transform-based cavityenhanced optical frequency comb spectroscopy that uses phase modulation at the cavity free spectral range frequency to achieve high sensitivity over broad spectral range.
  •  
41.
  • Johansson, Alexandra C., 1987-, et al. (author)
  • Optical frequency comb faraday rotation spectroscopy
  • 2018
  • In: 2018 Conference on Lasers and Electro-Optics, CLEO 2018 - Proceedings. - : Institute of Electrical and Electronics Engineers (IEEE). - 9781943580422 - 9781538657331
  • Conference paper (peer-reviewed)abstract
    • By combining Faraday rotation spectroscopy with an optical frequency comb Fourier transform spectrometer, we measure background- and calibration-free spectra of the entire Q- and R-branches of the fundamental band of nitric oxide at 1850-1920 cm-1.
  •  
42.
  • Johansson, Alexandra C., 1987- (author)
  • Optical Frequency Comb Fourier Transform Spectroscopy
  • 2018
  • Doctoral thesis (other academic/artistic)abstract
    • Fourier transform spectroscopy (FTS) based on optical frequency combs is an excellent spectroscopic tool as it provides broadband molecular spectra with high spectral resolution and an absolutely calibrated frequency scale. Moreover, the equidistant comb mode structure enables efficient coupling of the comb to enhancement cavities, yielding high detection sensitivity. This thesis focuses on further advances in comb-based FTS to improve its performance and extend its capabilities for broadband precision spectroscopy, particularly in terms of i) spectral resolution, ii) accuracy and precision of molecular parameters as well as concentrations retrieved from fitting models to spectra, and iii) species selectivity.To improve the spectral resolution we developed a new methodology to acquire and analyze comb-based FTS signals that yields spectra with a resolution limited by the comb linewidth rather than the optical path difference of the FTS, referred to as the sub-nominal resolution method. This method enables measurements of narrow features, e.g. low-pressure absorption spectra and modes of enhancement cavities, with frequency scale accuracy and precision provided by the comb. Using the technique we measured low-pressure spectra of the entire 3ν1+ν3 carbon dioxide (CO2) band at 1575 nm with sufficient signal-to-noise ratio and precision to observe collision narrowing of the absorption lineshape, which was for the first time with a comb-based spectroscopic technique. This allowed retrieval of spectral line parameters for this CO2 band using the speed-dependent Voigt profile.Using the sub-nominal resolution method, we measured the transmission modes of a Fabry-Perot cavity over 15 THz of bandwidth with kHz resolution and characterized the cavity modes in terms of their center frequency, linewidth, and amplitude. From the mode center frequencies, we retrieved the group delay dispersion of cavity mirror coatings and intracavity gas with an unprecedented combination of spectral bandwidth and resolution. By measuring both the mode broadening and frequency shift simultaneously we performed broadband cavity-enhanced complex refractive index spectroscopy (CE-CRIS), which allows for simultaneous and calibration-free assessment of the absorption and dispersion spectra of intracavity gas. In this first demonstration we measured the absorption and dispersion spectra of three combination bands of CO2 in the 1525 to 1620 nm range.Another comb-based FTS technique is noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS), which combines phase modulation and cavity-enhancement to obtain broadband and highly sensitive absorption spectra. In this thesis we improved the NICE-OFCS technique in terms of stability, sensitivity and modeling of the NICE-OFCS signal. We implemented a model of the NICE-OFCS signal with multiline fitting for assessment of gas concentration. We also identified the optimum operating conditions of the NICE-OFCS systems for accurate gas concentration assessment.Finally, to improve the species selectivity we combined comb-based FTS with the Faraday rotation spectroscopy (FRS) technique. In this first demonstration of optical frequency comb Faraday rotation spectroscopy (OFC-FRS), we measured background and interference-free spectra of the entire Q- and R-branches of the fundamental vibrational band of nitric oxide at 5.3 μm showing good agreement with the theoretical model.
  •  
43.
  • Johansson, Alexandra C., 1987-, et al. (author)
  • Precise comb-based fourier transform spectroscopy for line parameter retrieval
  • 2019
  • In: 2019 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference (CLEO/EUROPE-EQEC). - : Institute of Electrical and Electronics Engineers (IEEE). - 9781728104690
  • Conference paper (peer-reviewed)abstract
    • Accurate parameters of molecular transitions are needed for data analysis in many applications, ranging from atmospheric research to astrophysics and determination of fundamental constants. Optical frequency comb Fourier transform spectroscopy (OFC-FTS) is particularly well-suited for high-precision measurements of broadband molecular spectra. From these spectra, the parameters of individual transitions - all measured simultaneously under the same experimental conditions - can be determined. We use a mechanical OFC-FTS spectrometer with sub-nominal resolution [1, 2] to perform precise broadband measurements of entire molecular bands of CO2 using either direct absorption spectroscopy or cavity-enhanced complex refractive index spectroscopy (CE-CRIS) [3] and we extract line parameters for line shapes beyond the Voigt profile.
  •  
44.
  • Khodabakhsh, Amir, et al. (author)
  • Cavity-Enhanced Continuous-Filtering Vernier Spectroscopy at 3.3 mu m using a Femtosecond Optical Parametric Oscillator
  • 2017
  • In: 2017 CONFERENCE ON LASERS AND ELECTRO-OPTICS EUROPE &amp; EUROPEAN QUANTUM ELECTRONICS CONFERENCE (CLEO/EUROPE-EQEC). - : IEEE. - 9781509067367 ; , s. CH_2_2-
  • Conference paper (peer-reviewed)abstract
    • Optical frequency comb spectroscopy in the mid-infrared fingerprint region combines broad spectral bandwidth with high detection sensitivity and allows simultaneous detection of trace amounts of many molecular species. We have recently demonstrated a continuous-filtering Vernier spectrometer based on a mid-infrared optical frequency comb and an enhancement cavity for fast and sensitive detection of CH4 [1]. Here we present an improved, fully automatized and frequency calibrated continuous-filtering Vernier spectrometer, schematically shown in Fig. 1(a). The comb source is a doubly resonant optical parametric oscillator (DROPO) based on an orientation-patterned GaAs crystal synchronously pumped by a Tm:fiber femtosecond laser (125 MHz repetition rate, frep). The signal comb (3.1–3.4 µm, 30 mW) is mode matched to a 60-cm long Vernier enhancement cavity with a finesse of ~350 at 3.25 μm, placed in an enclosure that can be filled with the gas sample. The output mirror is attached to a PZT and mounted on a translation stage. When the cavity free spectral range is perfectly matched to twice the frep (250 MHz) every other signal comb mode is transmitted through the cavity. By detuning the cavity length from this perfect match position the cavity resonances act as a filter and transmit groups of comb modes called Vernier orders [2]. A diffraction grating mounted on a galvo-scanner separates these orders after the cavity and the chosen order is sent to the detection system. The Vernier order is tuned across the signal comb spectrum by scanning the cavity length (at 20 Hz) and the grating is rotated synchronously to fix the order in space and allow acquisition of the entire spectrum in 25 ms. Any residual mismatch between the cavity length scan and the grating rotation is compensated by a feedback loop acting on the frep of the pump laser and the PZT of the Vernier cavity [2]. A Fabry-Perot etalon is used for frequency calibration of the spectrometer. Figure 1(b) shows in black the normalized transmission spectrum of a sample containing 5.0 ppm CH4 and 160 ppm water. The red and blue curves show the corresponding fit of the Vernier spectrum [3] of CH4 and water, respectively, calculated using Voigt profiles, line parameters from the HITRAN database, and the experimentally determined cavity finesse. The figure of merit of the spectrometer is 1×10−9cm−1 Hz−1∕2 per spectral element and multiline fitting yields minimum detectable concentration of CH4 of 2 ppb in 25 ms, translating into 400 ppt Hz−1∕2 Since the spectrum of the signal comb covers the fundamental C-H stretch transitions we expect low detection limits for other hydrocarbons as well. In conclusion, mid-infrared comb-based continuous-filtering Vernier spectroscopy allows fast and highly sensitive measurement of broadband absorption spectra using a robust and compact detection system.
  •  
45.
  •  
46.
  • Khodabakhsh, Amir, et al. (author)
  • Fourier transform and vernier spectroscopy with a mid-infrared optical frequency comb
  • 2016
  • In: Light, energy and the environment. - : Optica Publishing Group (formerly OSA). - 9780960038046
  • Conference paper (peer-reviewed)abstract
    • We present a versatile frequency comb spectroscopy system based on a doubly resonant optical parametric oscillator tunable between 3-5.4 μm and two detection methods: a Fourier transform spectrometer and a continuous-filtering Vernier spectrometer.
  •  
47.
  • Khodabakhsh, Amir, et al. (author)
  • Near-infrared Fourier transform cavity-enhanced optical frequency comb spectroscopy
  • 2014
  • In: Fourier Transform Spectroscopy. - : OSA - The Optical Society. - 9780960038046 ; , s. 3-
  • Conference paper (peer-reviewed)abstract
    • Using Fourier transform-based cavity-enhanced optical frequency comb spectroscopy around 1.57 μm we measure high precision low pressure spectra of the 3v1+ v3 band of CO2 and high temperature H2O and OH spectra in a premixed methane/air flat flame.
  •  
48.
  • Khodabakhsh, Amir, et al. (author)
  • Noise-immune cavity-enhanced optical frequency comb spectroscopy
  • 2014
  • In: Optics Letters. - : Optical Society of America. - 0146-9592 .- 1539-4794. ; 39:17, s. 5034-5037
  • Journal article (peer-reviewed)abstract
    • We present a new method of optical frequency comb spectroscopy that combines cavity enhancement with frequency modulation to obtain immunity to laser frequency-to-amplitude noise conversion by the cavity modes and, thus, high absorption sensitivity over a broad spectral range. A frequency comb is locked to a cavity with a free spectral range (FSR) equal to 4/3 times the repetition rate of the laser, and phase-modulated at a frequency equal to the cavity FSR. The transmitted light is analyzed by a Fourier transform spectrometer with a high bandwidth detector. Phase-sensitive detection of the interferogram yields a noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) signal. In the first demonstration, we record NICE-OFCS signals from the overtone CO2 band at 1575 nm with absorption sensitivity of 4.3 x 10(-10) cm(-1) Hz(-1/2) per spectral element, close to the shot noise limit.
  •  
49.
  • Khodabakhsh, Amir, 1983-, et al. (author)
  • Noise-immune cavity-enhanced optical frequency comb spectroscopy : a sensitive technique for high-resolution broadband molecular detection
  • 2015
  • In: Applied physics. B, Lasers and optics (Print). - : Springer Berlin/Heidelberg. - 0946-2171 .- 1432-0649. ; 119:1, s. 87-96
  • Journal article (peer-reviewed)abstract
    • Noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) is a recently developed technique that utilizes phase modulation to obtain immunity to frequency-to-amplitude noise conversion by the cavity modes and yields high absorption sensitivity over a broad spectral range. We describe the principles of the technique and discuss possible comb-cavity matching solutions. We present a theoretical description of NICE-OFCS signals detected with a Fourier transform spectrometer (FTS) and validate the model by comparing it to experimental CO2 spectra around 1,575 nm. Our system is based on an Er:fiber femtosecond laser locked to a cavity and phase-modulated at a frequency equal to a multiple of the cavity free spectral range (FSR). The NICE-OFCS signal is detected by a fast-scanning FTS equipped with a high-bandwidth commercial detector. We demonstrate a simple method of passive locking of the modulation frequency to the cavity FSR that significantly improves the long-term stability of the system, allowing averaging times on the order of minutes. Using a cavity with a finesse of ~9,000, we obtain absorption sensitivity of 6.4 × 10−11 cm−1 Hz−1∕2 per spectral element and concentration detection limit for CO2 of 450 ppb Hz−1/2, determined by multiline fitting.
  •  
50.
  • Krzempek, Karol, et al. (author)
  • Compact 6.5 – 9 μm frequency comb source for fourier transform spectroscopy
  • 2020
  • In: Optics and Photonics for Sensing the Environment. - : The Optical Society. - 9781557528209
  • Conference paper (peer-reviewed)abstract
    • We demonstrate a compact fully-stabilized fiber-based optical frequency comb based on difference frequency generation tunable from 6.5 to 9 μm and its application to Fourier transform spectroscopy of nitrous oxide (N2O).
  •  
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