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Doppler-broadened NICE-OHMS beyond the cavity-limited weak absorption condition – I. Theoretical Description
Umeå University, Faculty of Science and Technology, Department of Physics. State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, Taiyuan 030006, China.
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.
2016 (English)In: Journal of Quantitative Spectroscopy and Radiative Transfer, ISSN 0022-4073, E-ISSN 1879-1352, Vol. 168, 217-244 p.Article in journal (Other academic) Published
Abstract [en]

Doppler-broadened (Db) noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) is conventionally described by an expression (here referred to as the CONV expression) that is restricted to the case when the single-pass absorbance, α0L, is much smaller than the empty cavity losses, π/F [here termed the conventional cavity-limited weak absorption (CCLWA) condition]. This limits the applicability of the technique, primarily its dynamic range and calibration capability. To remedy this, this work derives extended descriptions of Db NICEOHMS that are not restricted to the CCLWA condition. First, the general principles of Db NICEOHMS are scrutinized in some detail. Based solely upon a set of general assumptions, predominantly that it is appropriate to linearize the Beer–Lambert law, that the light is modulated to a triplet, and that the Pound–Drever–Hall sidebands are fully reflected, a general description of Db NICE-OHMS that is not limited to any specific restriction on α0L vs. π/F, here referred to as the FULL description, is derived. However, this description constitutes a set of equations to which no closed form solution has been found. Hence, it needs to be solved numerically (by iterations), which is inconvenient. To circumvent this, for the cases when α0Loπ/F but without the requirement that the stronger CCLWA condition needs to be fulfilled, a couple of simplified extended expressions that are expressible in closed analytical form, referred to as the extended locking and extended transmission description, ELET, and the extended locking and full transmission description, ELFT, have been derived. An analysis based on simulations validates the various descriptions and assesses to which extent they agree. It is shown that in the CCLWA limit, all extended descriptions revert to the CONV expression. The latter one deviates though from the extended ones for α0L around and above 0.1π/F. The two simplified extended descriptions agree with the FULL description for a larger range of α0L than the CONV expression, viz. for the ELET description for α0L up to 0.3π/F and for ELFT for α0L up to 0.6 or 1.0 π/F (depending on the mode of detection). It is then demonstrated that the conventional view of Db NICE-OHMS, which states that the out-of-phase and the in-phase signals can be referred to as a pure absorption and dispersion signal, respectively, breaks down when the CCLWA condition does not hold. In this case, the out-of-phase signal is additionally affected by the phase shifts of the laser components (i.e. dispersion) while the in-phase signal is also influenced by their attenuation. Access to new descriptions broadens considerably the dynamic range of Db NICE-OHMS and facilitates calibration using standard references samples, and thereby its applicability

Place, publisher, year, edition, pages
2016. Vol. 168, 217-244 p.
Keyword [en]
NICE-OHMS, Cavity enhanced spectroscopy, Dynamic range, Frequency modulation spectroscopy, Theoretical model
National Category
Atom and Molecular Physics and Optics
URN: urn:nbn:se:umu:diva-110271DOI: 10.1016/j.jqsrt.2015.09.007ISI: 000366007000018OAI: diva2:861900
Available from: 2015-10-19 Created: 2015-10-19 Last updated: 2016-03-14Bibliographically approved
In thesis
1. Cavity enhanced optical sensing
Open this publication in new window or tab >>Cavity enhanced optical sensing
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Kavitetsförstärkt optisk detektion
Abstract [en]

An optical cavity comprises a set of mirrors between which light can be reflected a number of times. The selectivity and stability of optical cavities make them extremely useful as frequency references or discri­mi­nators. With light coupled into the cavity, a sample placed inside a cavity will experience a significantly increased interaction length. Hence, they can be used also as amplifiers for sensing purposes. In the field of laser spectroscopy, some of the most sensitive techniques are therefore built upon optical cavities. In this work optical cavities are used to measure properties of gas samples, i.e. absorption, dispersion, and refractivity, with unprecedented precision.

The most sensitive detection technique of all, Doppler-broadened noise-immune cavity enhanced optical heterodyne molecular spectrometry (Db NICE-OHMS), has in this work been developed to an ultra-sensitive spectroscopic technique with unprecedented detection sensitivity. By identifying limiting factors, realizing new experimental setups, and deter­mining optimal detection conditions, the sensitivity of the technique has been improved several orders of magnitude, from 8 × 10-11 to 9 × 10-14 cm-1. The pressure interval in which NICE-OHMS can be applied has been extended by deri­vation and verification of dispersions equations for so-called Dicke narrowing and speed dependent broadening effects. The theoretical description of NICE-OHMS has been expanded through the development of a formalism that can be applied to the situations when the cavity absorption cannot be considered to be small, which has expanded the dynamic range of the technique. In order to enable analysis of a large number of molecules at their most sensitive transitions (mainly their funda­mental CH vibrational transitions) NICE-OHMS instrumentation has also been developed for measurements in the mid-infrared (MIR) region. While it has been difficult to realize this in the past due to a lack of optical modulators in the MIR range, the system has been based on an optical para­metric oscillator, which can be modulated in the near-infrared (NIR) range.

As the index of refraction can be related to density, it is possible to retrieve gas density from measurements of the index of refraction. Two such instru­men­tations have been realized. The first one is based on a laser locked to a measure­ment cavity whose frequency is measured by compassion with an optical frequency comb. The second one is based on two lasers locked to a dual-cavity (i.e. one reference and one measurement cavity). By these methods changes in gas density down to 1 × 10-9 kg/m3 can be detected.

All instrumentations presented in this work have pushed forward the limits of what previously has been considered measurable. The knowledge acquired will be of great use for future ultrasensitive cavity-based detection methods.

Place, publisher, year, edition, pages
Umeå: Umeå universitet, 2015. 124 p.
Optical resonators, Fiber Laser, Parametric oscillators, Optical frequency comb, Infrared, Spectroscopy heterodyne, Spectroscopy molecular, Absorption, Dispersion, Lineshapes, Optical standards and testing, Refractivety measurements
National Category
Atom and Molecular Physics and Optics
urn:nbn:se:umu:diva-110278 (URN)978-91-7601-338-0 (ISBN)
Public defence
2015-11-13, KBC-huset, KB3A9 (lilla hörsalen i KBC-huset), Umeå universitet, Umeå, 10:00 (English)
Swedish Research CouncilThe Kempe Foundations
Available from: 2015-10-23 Created: 2015-10-19 Last updated: 2015-10-29Bibliographically approved

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Ma, WeiguangSilander, IsakHausmaninger, ThomasAxner, Ove
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