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| 2. |
- Axner, Ove, 1957-, et al.
(författare)
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NICE-OHMS – frequency modulation cavity-enhanced spectroscopy : principles and performance
- 2014
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Ingår i: Cavity-Enhanced Spectroscopy and Sensing. - Berlin : Springer Berlin/Heidelberg. - 9783642400025 - 9783642400032 ; , s. 221-251
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Bokkapitel (refereegranskat)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.
(författare)
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Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry incorporating an optical circulator
- 2014
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Ingår i: Optics Letters. - : Optical Society of America. - 0146-9592 .- 1539-4794. ; 39:2, s. 279-282
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Tidskriftsartikel (refereegranskat)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.
(författare)
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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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Ingår i: Journal of the Optical Society of America. B, Optical physics. - 0740-3224 .- 1520-8540. ; 31:12, s. 2938-2945
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Tidskriftsartikel (refereegranskat)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. |
- Axner, Ove, 1957-, et al.
(författare)
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Noise-immune cavity-enhanced analytical atomic spectrometry — NICE-AAS : a technique for detection of elements down to zeptogram amounts
- 2014
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Ingår i: Spectrochimica Acta Part B - Atomic Spectroscopy. - : Elsevier. - 0584-8547 .- 1873-3565. ; 100, s. 211-235
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Tidskriftsartikel (refereegranskat)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) is a powerful technique for detection of molecular compounds in gas phase that is based on a combination of two important concepts: frequency modulation spectroscopy (FMS) for reduction of noise, and cavity enhancement, for prolongation of the interaction length between the light and the sample. Due to its unique properties, it has demonstrated unparalleled detection sensitivity when it comes to detection of molecular constituents in the gas phase. However, despite these, it has so far not been used for detection of atoms, i.e. for elemental analysis. The present work presents an assessment of the expected performance of Doppler-broadened (Db) NICE-OHMS for analytical atomic spectrometry, then referred to as noise-immune cavity-enhanced analytical atomic spectrometry (NICE-AAS). After a description of the basic principles of Db-NICE-OHMS, the modulation and detection conditions for optimum performance are identified. Based on a previous demonstrated detection sensitivity of Db-NICE-OHMS of 5×10−12 cm−1 Hz−1∕2 (corresponding to a single-pass absorbance of 7×10−11 over 10 s), the expected limits of detection (LODs) of Hg and Na by NICE-AAS are estimated. Hg is assumed to be detected in gas phase directly while Na is considered to be atomized in a graphite furnace (GF) prior to detection. It is shown that in the absence of spectral interferences, contaminated sample compartments, and optical saturation, it should be feasible to detect Hg down to 10 zg/cm3 (10 fg/m3 or 10-5 ng/m3), which corresponds to 25 atoms/cm3, and Na down to 0.5 zg (zg = zeptogram = 10-21 g), representing 50 zg/mL (parts-per-sextillion, pps, 1:1021) in liquid solution (assuming a sample of 10 µL) or solely 15 atoms injected into the GF, respectively. These LODs are several orders of magnitude lower (better) than any previous laser-based absorption technique previously has demonstrated under atmospheric pressure conditions. It is prophesied that NICE-AAS could provide such high detection sensitivity that the instrumentation should not, by itself, be the limiting factor of an assessment of elemental abundance; the accuracy of an assessment would then instead be limited by concomitant species, e.g. originating from the handling procedures of the sample or the environment.
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| 6. |
- Ehlers, Patrick, 1981-, et al.
(författare)
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Doppler broadened NICE-OHMS beyond the triplet formalism : assessment of optimum modulation index
- 2014
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Ingår i: Journal of the Optical Society of America. B, Optical physics. - : Optical Society of America. - 0740-3224 .- 1520-8540. ; 31:7, s. 1499-1507
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Tidskriftsartikel (refereegranskat)abstract
- The dependence of Doppler broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) on the modulation index, beta, has been investigated experimentally on C2H2 and CO2, both in the absence and the presence of optical saturation. It is shown that the maximum signals are obtained for beta that produce more than one pair of sidebands: in the Doppler limit and for the prevailing conditions (unsaturated transition and the pertinent modulation frequency and Doppler widths) around 1 and 1.4 for the dispersion and absorption detection phases, respectively. The results verify predictions given in an accompanying work. It is also shown that there is no substantial broadening of the NICE-OHMS signal for beta < 1. The use of beta of unity has yielded a Db-NICE-OHMS detection sensitivity of 4.9 x 10(-12) cm(-1) Hz(-1/2), which is the lowest (best) value so far achieved for NICE-OHMS based on a tunable laser. The number of sidebands that needs to be included in fits of the line-shape function to obtain good accuracy has been assessed. It is concluded that it is enough to consider three pairs of sidebands whenever the systematic errors in a concentration assessment should be below 1% when beta < 2 are used and <1 parts per thousand for beta < 1.5.
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| 7. |
- Ehlers, Patrick, 1981-, et al.
(författare)
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Doppler broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry : optimum modulation and demodulation conditions, cavity length, and modulation order
- 2014
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Ingår i: Journal of the Optical Society of America. B, Optical physics. - : The Optical Society of America. - 0740-3224 .- 1520-8540. ; 31:9, s. 2051-2060
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Tidskriftsartikel (refereegranskat)abstract
- Doppler broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry (Db-NICE-OHMS) has been scrutinized with respect to modulation and demodulation conditions (encompassing the modulation frequency,nu(m), the modulation index, beta, and the detection phase, theta), the cavity length, L, and the modulation order, k (defined as nu(m)/nu(FSR), where nu(FSR) is the free-spectral range of the cavity), primarily in the Doppler limit but also for two specific situations in the Voigt regime (for equal Doppler and homogeneous width and for purely Lorentzian broadened transitions), both in the absence and presence of optical saturation (the latter for the case in which the homogeneous broadening is smaller than the modulation frequency). It is found that, for a system with a given cavity length, the optimum conditions (i.e., those that produce the largest NICE-OHMS signal) for an unsaturated transition in the Doppler limit comprise nu(m)/Gamma(D) = 1.6 (where Gamma(D) is the half-width at half-maximum of the Doppler width of the transition), beta = 1.3, and theta = 0.78 pi. It is also found that the maximum is rather broad; the signal takes 95% of its maximum value for modulation frequencies in the entire 0.4 less than or similar to nu(m)/Gamma(D) less than or similar to 2.4 range. When optical saturation sets in, theta shifts toward the dispersion phase. The optimum conditions encompass k > 1 whenever L > 0.35L(D) and 2.6L(D) for the dispersion and absorption modes of detection, respectively [where L-D is a characteristic length given by c/(2 Gamma(D))]. Similar conditions are found under pressure broadened conditions.
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| 8. |
- Ehlers, Patrick, 1981-, et al.
(författare)
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Fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry instrumentation for Doppler-broadened detection in the 10-12 cm-1 Hz-1/2 region
- 2012
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Ingår i: Journal of the Optical Society of America. B, Optical physics. - : Optical Society of America. - 0740-3224 .- 1520-8540. ; 29:6, s. 1305-1315
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Tidskriftsartikel (refereegranskat)abstract
- A fiber-laser-based noise-immune cavity-enhanced optical heterodyne molecular spectrometry (FL-NICE-OHMS) system for white-noise-limited Doppler-broadened detection down to 5.6 x 10(-12) cm(-1) Hz(-1/2) is demonstrated. The system is based on a previous FL-NICE-OHMS instrumentation in which the locking of the laser frequency to a cavity mode has been improved by the use of an acousto-optic modulator (AOM) and provision of a more stable environment by the employment of a noise-isolating enclosed double-layer table, a temperature regulation of the laboratory, and an ultra-high-vacuum (UHV) gas system. White-noise behavior up to 10 s provides the instrument with a minimum detectable on-resonance absorbance per unit length of 1.8 x 10(-12) cm(-1) and a relative single-pass absorption (Delta I/I) of 7.2 x 10(-11). The system was applied to detection of acetylene on a transition at 1531.588 nm, yielding a detection sensitivity of C2H2 in atmospheric pressure gas of 4 ppt (measured over 10 s). (C) 2012 Optical Society of America
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| 9. |
- Ehlers, Patrick, 1981-
(författare)
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Further development of NICE-OHMS : – an ultra-sensitive frequency-modulated cavity-enhanced laser-based spectroscopic
technique for detection of molecules in gas phase
- 2014
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Noise-immune cavity-enhanced optical heterodyne molecular spectroscopy, NICE-OHMS, is a laser-based spectroscopic detection technique that comprises the concepts of frequency modulation (FM, for reduction of 1/f-noise by detecting the signal at a high frequency) and cavity enhancement (CE, for a prolongation of the optical path length) in a unique way. Properly designed, this gives the technique an intrinsic immunity against the frequency-to-noise conversion that limits many other types of CE techniques. All this gives it an exceptionally high sensitivity for detection of molecular species. Although originally developed for frequency standard purposes in the late 1990s, soon thereafter development of the technique towards molecular spectroscopy and trace gas detection was initiated. This thesis focuses on the further development of Doppler- broadened NICE-OHMS towards an ultra-sensitive detection technique. A number of concepts have been addressed. A few of these are: i) The detection sensitivity of fiber-laser-based NICE- OHMS has been improved to the 10−12 cm−1 range, which for detection of C2H2 corresponds to a few ppt (parts-per-trillion, 1:1012) in gas phase, by improving the locking of the laser to a cavity mode by use of an acousto-optic modulator. ii) It is shown that the system can be realized with a more compact footprint by implementation of a fiber-optic circulator. iii) A systematic and thorough investigation of the experimental conditions that provide maximum signals, referred to as the optimum conditions, e.g. modulation and demodulation conditions and cavity length, has been performed. As a part of this, an expression for the NICE-OHMS line shape beyond the conventional triplet formalism has been proposed and verified. iv) To widen the applicability of NICE-OHMS for detection of pressure broadened signals, also a setup based upon a distributed-feedback (DFB) laser has been realized. v) In this regime, the Voigt profile cannot model signals with the accuracy that is needed for a proper assessment of analyte concentrations. Therefore, the thesis demonstrates the first implementations of line profiles encompassing Dicke narrowing and speed-dependent effects to NICE-OHMS. While such profiles are well-known for absorption, there were no expressions available for their dispersion counterparts. Such expressions have been derived and validated by accompanying experiments. vi) The applicability of the technique for elemental detection, then referred to as NICE-AAS, has been prophesied.
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| 10. |
- Silander, Isak, 1980-, et al.
(författare)
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Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry down to 4 x 10-13 cm-1 Hz-1/2 : implementation of a 50,000 finesse cavity
- 2015
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Ingår i: Optics Letters. - : Optical Society of America. - 0146-9592 .- 1539-4794. ; 40:9, s. 2004-2007
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Tidskriftsartikel (refereegranskat)abstract
- We report on the realization of a Doppler-broadened noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) instrumentation based on a high-finesse (50,000) cavity with a detection sensitivity of 4 x 10(-13) cm(-1) Hz(-1/2). For the P-e(11) transition targeted at 1.5316 mu m, this corresponds to a C2H2 concentration of 240 ppq (parts-per-quadrillion) detected at 100 Torr. The setup was originally affected by recurrent dips in the cavity transmission, which were attributed to excitation of high-order transverse mode by scattering from the mirrors. The effect of these was reduced by insertion of a small pinhole in the cavity.
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