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High resolution ultra-sensitive trace gas detection by use of cavity-position-modulated sub-Doppler NICE-OHMS - Application to detection of acetylene in human breath
Umeå University, Faculty of Science and Technology, Department of Physics. State Key Laboratory of Quantum Optics & Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, 030006 Taiyuan, China; Collaborative Innovation Center of Extreme Optics, Shanxi University, 030006 Taiyuan, China.ORCID iD: 0000-0002-3966-8943
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Applied Physics and Electronics.ORCID iD: 0000-0002-5065-7786
State Key Laboratory of Quantum Optics & Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, 030006 Taiyuan, China; Collaborative Innovation Center of Extreme Optics, Shanxi University, 030006 Taiyuan, China.
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

A sensitive high resolution spectrometer for trace gas detection of species whose transitions have severe spectral overlap with abundant concomitant species by sub-Doppler (sD) noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) is presented. The setup is based on a NICE-OHMS instrumentation utilizing balanced detection that provides shot-noise limited Doppler-broadened (Db) detection. An additional layer of modulation is added to reduce the influence of narrow etalons and improve the sensitivity for sD detection. By dithering synchronously the positions of the two cavity mirrors, the effect of residual etalons between one of the cavity mirrors and another surface in the system could be reduced without affecting the frequencies of the cavity mode. This reduced the drifts in the system, allowing for an Allan deviation of the absorption coefficient of 2.2×10−13 cm−1 for an integration time of 60 s, which, for the targeted C2H2 transition at 6518.4858 cm−1, corresponds to a 3σ detection sensitivity of 130 ppt. Sub-Doppler trace gas detection is demonstrated by measuring ppb levels of C2H2 in the exhaled breath of smokers. A procedure was worked out for simultaneous detection of CO2, based on the Db response. It is shown that despite significant spectral interference from CO2, which precludes Db detection of C2H2 in breath, acetylene could be detected in breath from smokers with good spectral resolution by the use of sD NICE-OHMS.

National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:umu:diva-153065OAI: oai:DiVA.org:umu-153065DiVA, id: diva2:1261003
Available from: 2018-11-06 Created: 2018-11-06 Last updated: 2018-11-07
In thesis
1. Mid- and near-infrared NICE-OHMS: techniques for ultra-sensitive detection of molecules in gas phase
Open this publication in new window or tab >>Mid- and near-infrared NICE-OHMS: techniques for ultra-sensitive detection of molecules in gas phase
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Noise-immune cavity-enhanced optical heterodyne molecular spectrometry (NICE-OHMS) is a technique for ultra-sensitive detection of molecular absorption and dispersion. For highest performance, the technique combines cavity enhancement (CE) with frequency modulation (FM); while the former increases the effective interaction length between the light and the analyte by several orders of magnitudes, the latter removes the in-coupling of 1/f noise and makes the signals background free. The combination of CE and FM also gives the technique an immunity to amplitude noise caused by the jitter of the laser frequency relative to the cavity resonance frequencies. All these properties make the technique suitable for ultra sensitive trace gas detection in the sub-parts-per-trillion (ppt) range. The aim of this thesis is to improve the performance of the NICE-OHMS technique and to increase its range of applications.

The work in this thesis can be divided into three areas:Firstly, a mid-infrared (MIR)-NICE-OHMS instrumentation was developed. In a first realization an unprecedented white-noise equivalent absorption limit for Doppler broadened (Db) detection in the MIR of 3×10-9 cm-1Hz-1/2was demonstrated. This was subsequently improved to 2.4×10-10 cm-1Hz-1/2allowing for detection methane and its two main isotopologues (CH3D and 13CH4) at their natural abundance.Secondly, further development of an existing near-infrared NICE-OHMS system was performed. This resulted in an improved longtime stability and the first shot-noise limited NICE-OHMS system for Db detection with a noise equivalent absorption limit of 2.3×10-14 cm-1detected over 200 s. Thirdly, models and theoretical descriptions of NICE-OHMS signals under strong absorption conditions and from methane under high laser power were developed. It was experimentally verified that the models allow for a more accurate evaluation of NICE-OHMS signals under a wide range of conditions.

Abstract [sv]

Brusimmun kavitetsförstärkt optisk-heterodyndetekterad molekylärspektroskopi (eng.Noise-immune cavity-enhanced optical heterodyne molecular spectrometry, NICE-OHMS) är en teknik för ultrakänslig detektion av molekylär absorption och dispersion. NICE-OHMS-tekniken kombinerar kavitetsförstärkning (eng. CE) med frekvensmodulering (FM); emedan den första väsentligt ökar den effektiva interaktionslängden mellan ljuset och analyten vilket ökar teknikens känslighet, tar den senare bort inkopplingen av 1/f-brus och gör signalerna bakgrundsfria. Kombinationen av CE och FM ger också tekniken en immunitet mot amplitudstörning som orsakas av jitter hos laserljusets frekvens i förhållande till kavitetsresonansfrekvenserna. Alla dessa egenskaper gör tekniken lämplig för ultrakänslig spårgasdetektering i och under ppt (eng. parts-per-trillion) - området. Syftet med denna avhandling är att förbättra prestandan hos NICE-OHMS-tekniken och att öka dess tillämpningspotential.

Avhandlingen kan delas in i tre delar: Inom den första utvecklades en mid-infraröd (MIR)-NICE-OHMS instrumentering. Vid en första realisering påvisades en aldrig tidigare uppnådd vitt-brus-ekvivalent absorptionsgräns för Dopplerbreddad (Db) detektering i MIR området på 3 × 10-9 cm-1Hz-1/2. Detta förbättrades därefter till 2,4 x 10-10 cm-1Hz-1/2, vilket möjliggör detektering av metan och dess två huvudsakliga isotopologer (CH3D och 13CH4) vid deras naturliga förekomst. Inom det andra området utfördes vidareutveckling av ett existerande NICE-OHMS-system verksamt i det när-infraröda (NIR) området. Detta resulterade i en förbättrad långtidsstabilitet och en brus-ekvivalent absorptionsgräns för Db detektion på 2,3 × 10-14 cm-1 mätt över 200 s. Inom den tredje utvecklades modeller och teoretiska beskrivningar av NICE-OHMS under starka absorptionsförhållanden och från metan under hög laserintensitet. Det var experimentellt verifierat att modellerna möjliggör en mer noggrann utvärdering av NICE-OHMS-signalerunder ett stort antal förhållanden.

Place, publisher, year, edition, pages
Umeå: Umeå universitet, 2018. p. 139
Keywords
spectrometry, NICE-OHMS, trace gas detection, acetylene, methane, isotopologues, near-infrared, mid-infrared, shot-noise, optical parametric oscillator
National Category
Atom and Molecular Physics and Optics
Research subject
Technical Physics
Identifiers
urn:nbn:se:umu:diva-153068 (URN)978-91-7601-977-1 (ISBN)
Public defence
2018-11-30, N450, Naturvetarhuset, Umeå, 10:00 (English)
Opponent
Supervisors
Available from: 2018-11-09 Created: 2018-11-06 Last updated: 2018-11-13Bibliographically approved

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Zhao, GangHausmaninger, ThomasSchmidt, Florian M.Axner, Ove

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