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Wavelength modulation absorption spectrometry from optically saturated collision-broadened transitions
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Physics.
2005 (English)In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 94, no 2, 225-254 p.Article in journal (Refereed) Published
Abstract [en]

A theoretical investigation of the influence of optical saturation on wavelength modulation absorption spectrometry (WMAS) signals from collision-broadened transitions is presented. Expressions are derived for the nth Fourier coefficient of the analytical detector signal, and thereby also for the nth harmonic signal from a WMAS instrumentation (i.e. the nf-WMAS signal), from a wavelength modulated collision-broadened transition exposed to optical saturation. The flux- (or irradiance-) and modulation-amplitude dependences of the nf-WMAS signal on resonance are scrutinized in detail. It is shown that the nth Fourier coefficient of the wavelength modulated analytical detector signal from an optically saturated collision-broadened transition can be written as a product of a flux-dependent (φ) bleaching function, given by (1+φ/φsat)-1 and identical to that appearing for ordinary, unmodulated absorption spectrometry (AS), and a flux-, detuning-, and modulation-amplitude-dependent wavelength modulated peak-normalized saturation-broadened Lorentzian lineshape function, specific for the WMAS technique. It is found that the nf-WMAS signal on resonance decreases faster than an ordinary AS signal as a function of laser flux when smaller-than-optimum modulation amplitudes are used, but slower when larger-than-optimum modulation amplitudes are used. When optimum (or close-to-optimum) modulation amplitudes are being used, on the other hand, the flux dependence of the WMAS signal resembles to a large degree that of ordinary AS. The conditions for when WMAS from collision-broadened transitions has the same flux dependence as ordinary AS are identified.

Place, publisher, year, edition, pages
Oxford: Pergamon Press , 2005. Vol. 94, no 2, 225-254 p.
Keyword [en]
Wavelength modulation, Diode laser, Absorption spectrometry, WMS, WMAS, Optical saturation, Bleaching
URN: urn:nbn:se:umu:diva-11933DOI: 10.1016/j.jqsrt.2004.09.010OAI: diva2:151604
Available from: 2008-01-16 Created: 2008-01-16 Last updated: 2013-01-30
In thesis
1. Laser-based absorption spectrometry: development of NICE-OHMS towards ultra-sensitive trace species detection
Open this publication in new window or tab >>Laser-based absorption spectrometry: development of NICE-OHMS towards ultra-sensitive trace species detection
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Laser-based absorption spectroscopy (AS) is a powerful technique for qualitative and quantitative studies of atoms and molecules. An important field of use of AS is the detection of species in trace concentrations, which has applications not only in physics and chemistry but also in biology and medicine, encompassing environmental monitoring, regulation of industrial processes and breath analysis. Although a large number of molecular species can successfully be detected with established AS techniques, there are some applications that require higher sensitivity, selectivity and accuracy, yet robust and compact instrumentation.

Various approaches have been made during the years to improve on the performance of AS, usually based on modulation spectrometry or external cavities. The most sensitive absorption technique of today is, however, noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS). This technique elegantly combines several approaches: external cavities (for optical path length enhancement), modulation techniques (for noise reduction) and saturation spectroscopy (for enhanced selectivity). However, due to its complexity, the technique has so far not been applied to practical trace species detection.

This thesis provides the background for an understanding of NICE-OHMS and describes the construction of a first compact NICE-OHMS spectrometer based on a narrowband fiber laser. Moreover, it gives theoretical expressions for NICE-OHMS signal lineshapes, measured in various modes of detection, which can be fitted to the experimental data and thereby facilitate the assessment of species concentration. The sensitivity of the instrumentation is demonstrated by detection of acetylene (C2H2) and carbon dioxide (CO2) in the 1.5 μm region. A fractional absorption sensitivity of 3*10-9 (integrated absorption of 5*10-11 cm-1), could be achieved using a cavity with a finesse of 4800 and an acquisition time of 0.7 s. This results in a detection limit for C2H2 of 4.5 ppt (4.5*10-12 atm).

In addition, the thesis revives the idea of using an accurate (frequency) measurement of the free-spectral-range (FSR) of an external cavity for sensitive and calibration-free concentration assessment. A theoretical description of the expected signal lineshapes is given, and in a first experimental demonstration the FSR could be measured with a resolution of 5 Hz, resulting in a fractional absorption sensitivity of 1*10-7, and subsequently in a detection limit for C2H2 of 180 ppt (12.5 s acquisition time).

The thesis, finally, also contributes to the continuously ongoing development of conventional AS and wavelength modulated AS by addressing concepts related to when the light optically saturates the transition.

Place, publisher, year, edition, pages
Umeå: Fysik, 2007. 91 p.
absorption spectrometry, trace species detection, fiber laser, modulation, cavity-enhanced spectroscopy, optical saturation, laser frequency stabilization, free-spectral-range
National Category
Physical Sciences
urn:nbn:se:umu:diva-1414 (URN)978-91-7264-403-8 (ISBN)
Public defence
2007-11-23, N430, Naturvetarhuset, Umeå Universitet Campus, Umeå, 13:15
Available from: 2007-11-01 Created: 2007-11-01 Last updated: 2013-01-31Bibliographically approved

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Schmidt, FlorianFoltynowicz, AleksandraGustafsson, JörgenAxner, Ove
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