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  • 1. Kluczynski, P.
    et al.
    Jahjah, M.
    Naehle, L.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Belahsene, S.
    Fischer, M.
    Koeth, J.
    Rouillard, Y.
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Vicet, A.
    Lundqvist, S.
    Detection of acetylene impurities in ethylene and polyethylene manufacturing processes using tunable diode laser spectroscopy in the 3-mu m range2011In: Applied physics. B, Lasers and optics (Print), ISSN 0946-2171, E-ISSN 1432-0649, Vol. 105, no 2, p. 427-434Article in journal (Refereed)
    Abstract [en]

    Using recently developed GaInAsSb/AlGaInAsSb DFB lasers, tunable diode laser spectroscopy (TDLS) has been extended into the 3-mu m wavelength region for the detection of acetylene impurities in hydrocarbon compounds encountered in ethylene manufacturing. Measurements of acetylene in pure polymer grade ethylene and in a gas mixture of ethylene and ethane typical of the process stream around a hydrogenation reactor have been performed. Using a procedure incorporating subtraction of a hydrocarbon background spectrum a detection limit of 5 ppb m was achieved under ordinary laboratory conditions. Under forced temperature cycling conditions, the detection limit deteriorated to 180 ppb m, due to temperature drift caused by optical interferences generated by reflections in the laser TO8 can.

  • 2. Kluczynski, Pawel
    et al.
    Lundqvist, Stefan
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Faraday rotation spectrometer with sub-second response time for detection of nitric oxide using a cw DFB quantum cascade laser at 5.33 µm2011In: Applied physics. B, Lasers and optics (Print), ISSN 0946-2171, E-ISSN 1432-0649, Vol. 103, no 2, p. 451-459Article in journal (Refereed)
    Abstract [en]

    A Faraday modulation spectrometer for sensitive and fast detection of nitric oxide at 5.33 μm utilizing a room temperature continuous wave distributed feedback quantum cascade laser and a Peltier cooled MCT detector is presented. The magnetic field was modulated at 7.4 kHz whereas the laser wavelength was scanned at 20 Hz across the most favorable rotational-vibrational transition for FAMOS, Q3/2(3/2), at 5.33 μm. Using a 15 cm optical path and lineshape fitting, the spectrometer provides a detection limit of 4.5 ppb for a response time of 1 s. An Allan variance analysis demonstrates that the system has an excellent stability, up to several hours of operation.

  • 3.
    Lathdavong, Lemthong
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Shao, Jie
    Institute of Information Optics of Zhejiang Normal University.
    Dion, Claude M.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kluczynski, Pawel
    Siemens AB.
    Lundqvist, Stefan
    Siemens AB.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Faraday modulation spectrometry of nitric oxide addressing its electronic X2Π − A2Σ+ band: I. theory2010In: Applied Optics, ISSN 1559-128X, E-ISSN 2155-3165, Vol. 49, no 29, p. 5597-5613Article in journal (Refereed)
    Abstract [en]

    We give a simple two-transition model of Faraday modulation spectrometry (FAMOS) addressing the electronic X2Π(ν''=0) − A2Σ+(ν'=0) band in nitric oxide. The model is given in terms of the integrated line strength, S, and first Fourier coefficients for the magnetic-field-modulated dispersive line shape function. Although the two states addressed respond differently to the magnetic field (they adhere to the dissimilar Hund coupling cases), it is shown that the technique shares some properties with FAMOS when rotational-vibrational Q-transitions are targeted: the line shapes have a similar form and the signal strength has an analogous magnetic field and pressure dependence. The differences are that the maximum signal appears for larger magnetic field amplitudes and pressures, ∼1500 G and ∼200 Torr, respectively.

  • 4.
    Shao, Jie
    et al.
    Institute of Information Optics of Zhejiang Normal University.
    Lathdavong, Lemthong
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kluczynski, Pawel
    Siemens AB.
    Lundqvist, Stefan
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Faraday modulation spectrometry of nitric oxide addressing its electronic X2Π - A2Σ+ band: II. experiment2010In: Applied Optics, ISSN 1559-128X, E-ISSN 2155-3165, Vol. 49, no 29, p. 5614-5625Article in journal (Refereed)
    Abstract [en]

    A first demonstration of Faraday modulation spectrometry (FAMOS) of nitric oxide (NO) addressing its strong electronic X2Π(ν″=0)−A2Σ+=0) band is presented. The instrumentation was constructed around a fully diode-laser-based laser system producing mW powers of ultraviolet light targeting the overlapping Q22(21/2) and R12Q(21/2) transitions at ∼226.6nm. The work verifies a new two-transition model of FAMOS addressing the electronic transitions in NO given in an accompanying work. Although the experimental instrumentation could address neither the parameter space of the theory nor the optimum conditions, the line shapes and the pressure dependence could be verified under low-field conditions. NO could be detected down to a partial pressure of 13µTorr, roughly corresponding to 10ppb·m for an atmospheric pressure sample, which demonstrates the feasibility of FAMOS for sensitive detection of NO addressing its strong electronic band. A first demonstration of Faraday modulation spectrometry (FAMOS) of nitric oxide (NO) addressing its srtong electronic X2Π - A2Σ+ band is presented. The instrumentation was constructed around a fully diode-laser-based laser system producing mW powers of ultraviolet light targeting the overlapping Q22(21) and QR12(21) transitions at around 226.6 nm. The work verifies a new two-transition model of FAMOS addressing the electronic transitions in NO given in an accompanying work. Although the experimental instrumentation could address neither the parameter space of the theory nor the optimum conditions, the line shapes and the pressure dependence could be verified under low-field conditions. NO could be detected down to a partial pressure of 13 μTorr, roughly corresponding to 10 ppb · mfor an atmospheric pressure sample, which demonstrates the feasibility of FAMOS for sensitive detection of NO addressing its strong electronic band.

  • 5.
    Wang, Junyang
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Ehlers, Patrick
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Silander, Isak
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Speed-dependent Voigt dispersion line-shape function: applicable to techniques measuring dispersion signals2012In: Journal of the Optical Society of America. B, Optical physics, ISSN 0740-3224, E-ISSN 1520-8540, Vol. 29, no 10, p. 2971-2979Article in journal (Refereed)
    Abstract [en]

    An analytical expression for a Voigt dispersion line-shape function that incorporates speed-dependent effects (SDEs) on the collision broadening, applicable to spectroscopic techniques that measure dispersion signals, is presented. It is based upon a speed-dependent Voigt (SDV) model for absorption spectrometry that assumes that the molecular relaxation rate has a quadratic dependence on molecular speed. The expression is validated theoretically in the limit of small SDEs by demonstration that it reverts to the ordinary Voigt dispersion line-shape function and experimentally in a separate work by experiments performed by the noise-immune cavity-enhanced optical heterodyne molecular spectrometry technique. A comparison is given between the SDEs in the SDV absorption and dispersion line-shape functions. It is shown that both line shapes are affected significantly but differently by SDEs. The expression derived provides, for the first time to our knowledge, a possibility also for the techniques that measure dispersion signals to handle SDEs. (c) 2012 Optical Society of America

  • 6.
    Westberg, Jonas
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Faraday modulation spectroscopy: Theoretical description and experimental realization for detection of nitric oxide2013Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Faraday modulation spectroscopy (FAMOS) is a laser-based spectroscopic dispersion technique for detection of paramagnetic molecules in gas phase. This thesis presents both a new theoretical description of FAMOS and experimental results from the ultra-violet (UV) as well as the mid-infrared (MIR) regions. The theoretical description, which is given in terms of the integrated linestrength and Fourier coefficients of modulated dispersion and absorption lineshape functions, facilitates the description and the use of the technique considerably. It serves as an extension to the existing FAMOS model that thereby incorporates also the effects of lineshape asymmetries primarily originating from polarization imperfections. It is shown how the Fourier coefficients of modulated Lorentzian lineshape functions, applicable to the case with fully collisionally broadened transitions, can be expressed in terms of analytical functions. For the cases where also Doppler broadening needs to be included, resulting in lineshapes of Voigt type, the lineshape functions can be swiftly evaluated (orders of magnitude faster than previous procedures) by a newly developed method for rapid calculation of modulated Voigt lineshapes (the WWA-method). All this makes real-time curve fitting to FAMOS spectra feasible. Two experimental configurations for sensitive detection of nitric oxide (NO) by the FAMOS technique are considered and their optimum conditions are determined. The two configurations target transitions originating from the overlapping Q22(21=2) and QR12(21=2) transitions in the ultra-violet (UV) region (227nm) and the Q3=2(3=2)-transition in the fundamental rotational-vibrational band in the mid-infrared (MIR) region (5.33 µm). It is shown that the implementations of FAMOS in the UV- and MIR-region can provide detection limits in the low ppb range, which opens up the possibility for applications where high detection sensitivities of NO is required.

  • 7.
    Westberg, Jonas
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Lineshape asymmetries in Faraday modulation spectroscopy2014In: Applied physics. B, Lasers and optics (Print), ISSN 0946-2171, E-ISSN 1432-0649, Vol. 116, no 2, p. 467-476Article in journal (Refereed)
    Abstract [en]

    Faraday modulation/rotation spectroscopy (FAMOS/FRS) is a spectroscopic technique for detection of paramagnetic species in gas phase. Although the prevailing theoretical description predicts fully symmetrical lineshapes, experiments do not in general provide such. This work shows that asymmetries in FAMOS can have at least two origins; (i) a frequency dependent laser intensity and (ii) polarization imperfections, which both are scrutinized here. A general analytical description for the latter, derived under the assumption that both the polarization imperfections and the relative absorption are small, is presented, conveniently expressed in terms of 1st Fourier coefficients of modulated dispersion and absorption lineshape functions. The resulting expression, which is thus an extension to the conventional FAMOS expression, can thereby be swiftly evaluated and allows for on-line fitting to measured asymmetric FAMOS signals. Curve fits to experimentally obtained data from nitric oxide measured both in the ultra-violet and the mid-infrared region demonstrate the applicability of the methodology.

  • 8.
    Westberg, Jonas
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Kluczynski, Pawel
    Lundqvist, Stefan
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Analytical expression for the nth Fourier coefficient of a modulated Lorentzian dispersion lineshape function2011In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 112, no 9, p. 1443-1449Article in journal (Refereed)
    Abstract [en]

    Modulated spectroscopic detection techniques that rely on dispersion, e.g. Faraday modulation/rotation spectroscopy and wavelength-modulated noise-immune cavity-enhanced optical heterodyne molecular spectroscopy, are often described in terms of Fourier coefficients of a modulated dispersion lineshape function. This work derives a non-complex analytical expression for the nth Fourier coefficient of a modulated Lorentzian dispersion lineshape function. The expression is easier to implement, and orders of magnitude faster to execute, than previous approaches involving numerical calculations of integrals. The first six Fourier coefficients are explicitly given and illustrated for their optimum modulation amplitudes, which are also given

  • 9.
    Westberg, Jonas
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Lathdavong, Lemthong
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Dion, Claude M.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Shao, Jie
    Institute of Information Optics of Zhejiang Normal University, Jinhua, China.
    Kluczynski, Pawel
    Siemens AB, Göteborg, Sweden.
    Lundqvist, Stefan
    Siemens AB, Göteborg, Sweden.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Quantitative description of Faraday modulation spectrometry in terms of the integrated linestrength and 1st Fourier coefficients of the modulated lineshape function2010In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 111, no 16, p. 2415-2433Article in journal (Refereed)
    Abstract [en]

    A quantitative description of the strength and shape of Faraday modulation spectrometry (FAMOS) signals is given. It is first shown how the signal can be expressed in terms of the integrated linestrength for the targeted transition, Si,j. Secondly, since the technique relies on a periodic modulation of the transition frequency induced by an alternating magnetic field, it is explicitly shown that it is possible to express the FAMOS signal concisely in terms of 1st Fourier coefficients of a magnetic-field-modulated dispersive lineshape function for left- and right-handed circularly polarized light. Expressions for the FAMOS signal in terms of the integrated linestrength and such Fourier coefficients are given for three cases: (i) for transitions between two arbitrary types of states, (ii) for transitions between two states that both belong to Hund’s coupling case (a), as is the case for rotational–vibrational transitions of NO, and finally (iii) for the commonly used Q-transitions between such states. It is finally shown that the FAMOS signal from a Q-transition can be expressed succinctly solely in terms of one 1st Fourier coefficient. A general analysis of FAMOS addressing an arbitrary Q-transition as well as the most sensitive Q3/2(3/2) transition in NO is given. The conditions for maximum signal are specifically identified.

  • 10.
    Westberg, Jonas
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wang, Junyang
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Fast and non-approximate methodology for calculation of wavelength-modulated Voigt lineshape functions suitable for real-time curve fitting2012In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 113, no 16, p. 2049-2057Article in journal (Refereed)
    Abstract [en]

    Wavelength modulation (WM) produces lock-in signals that are proportional to various Fourier coefficients of the modulated lineshape function of the molecular transition targeted. Unlike the case for the Lorentzian lineshape function, there is no known analytical expression for the Fourier coefficients of a modulated Voigt lineshape function; they consist of nested integrals that have to be solved numerically, which is often time-consuming and prevents real-time curve fitting. Previous attempts to overcome these limitations have so far consisted of approximations of the Voigt lineshape function, which brings in inaccuracies. In this paper we demonstrate a new means to calculate the lineshape of nf-WM absorption signals from a transition with a Voigt profile. It is shown that the signal can conveniently be expressed as a convolution of one or several Fourier coefficients of a modulated Lorentzian lineshape function, for which there are analytical expressions, and the Maxwell-Boltzmann velocity distribution for the system under study. Mathematically, the procedure involves no approximations, wherefore its accuracy is limited only by the numerical precision of the software used (in this case similar to 10(-16)) while the calculation time is reduced by roughly three orders of magnitude (10(-3)) as compared to the conventional methodology, i.e. typically from the second to the millisecond range. This makes feasible real-time curve fitting to lock-in output signals from modulated Voigt profiles. (C) 2012 Elsevier Ltd. All rights reserved.

  • 11.
    Westberg, Jonas
    et al.
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Wang, Junyang
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Axner, Ove
    Umeå University, Faculty of Science and Technology, Department of Physics.
    Methodology for fast curve fitting to modulated Voigt dispersion lineshape functions2014In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 133, p. 244-250Article in journal (Refereed)
    Abstract [en]

    Faraday rotation spectroscopy (FAMOS) as well as other modulated techniques that rely on dispersion produce lock-in signals that are proportional to various Fourier coefficients of modulated dispersion lineshape functions of the molecular transition targeted. In order to enable real-time curve fitting to such signals a fast methodology for calculating the Fourier coefficients of modulated lineshape functions is needed. Although there exist an analytical expression for such Fourier coefficients of modulated Lorentzian absorption and dispersion lineshape functions, there is no corresponding expression for a modulated Voigt dispersion function. The conventional computational route of such Fourier coefficients has therefore so far either consisted of using various approximations to the modulated Voigt lineshape function or solving time-consuming integrals, which has precluded accurate real-time curve fitting. Here we present a new methodology to calculate Fourier coefficients of modulated Voigt dispersion lineshape functions that is significantly faster (several orders of magnitude) and more accurate than previous approximative calculation procedures, which allows for real-time curve fitting to FAMOS signals also in the Voigt regime.

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