Abstract

An efficient method for the detection of acetone, an important biomarker in exhaled breath, by utilizing wavelength modulation spectroscopy (WMS) with a mid-infrared distributed feedback interband cascade laser (DFB-ICL) is presented. The performance of the DFB-ICL laser is characterized, and its linewidth is measured to be $\mbox{(3}.\mbox{39} \pm 0.\mbox{15)}$ MHz by beating the output with an auxiliary mid-IR frequency comb over 50 ms. The measured asymmetric acetone absorption profile with the center wavelength around 3367 nm is fitted by the pseudo-Voigt function. The phase shift between the intensity and frequency modulations is determined and used for processing the results. The sensor is tested by performing measurements with calibration mixtures of acetone in nitrogen, and the detection limits of 0.58 ppm and 0.12 ppm were determined with 1 s and 60 s signal averaging times, respectively. Our work shows that wavelength modulation spectroscopy with a DFB-ICL laser complimented by a multipass cell for higher sensitivity can be efficiently used for acetone detection and is promising for sensitive breath analysis.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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    [Crossref]
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    [Crossref]

2018 (4)

B. Henderson, A. Khodabakhsh, M. Metsälä, I. Ventrillard, F. M. Schmidt, D. Romanini, G. A. D. Ritchie, S. t. L. Hekkert, R. Briot, T. Risby, N. Marczin, F. J. M. Harren, and S. M. Cristescu, “Laser spectroscopy for breath analysis: towards clinical implementation,” Appl. Phys. B 124(8), 161 (2018).
[Crossref]

F. Nadeem, J. Mandon, A. Khodabakhsh, S. M. Critescu, and F. J. M. Harren, “Sensitive Spectroscopy of Acetone Using a Widely Tunable External-Cavity Quantum Cascade Laser,” Sensors 18(7), 2050 (2018).
[Crossref]

A. Bicer, J. Bounds, F. Zhu, A. A. Kolomenski, N. Kaya, E. Aluauee, M. Amani, and H. A. Schuessler, “Sensitive Spectroscopic Analysis of Biomarkers in Exhaled Breath,” Int. J. Thermophys. 39(6), 69 (2018).
[Crossref]

J. Y. Li, G. Luo, Z. H. Du, and Y. W. Ma, “Hollow waveguide enhanced dimethyl sulfide sensor based on a 3.3 um interband cascade laser,” Sens. Actuators B 255, 3550–3557 (2018).
[Crossref]

2017 (3)

J. B. Xia, F. Zhu, S. S. Zhang, A. Kolomenskii, and H. Schuessler, “A ppb level sensitive sensor for atmospheric methane detection,” Infrared Phys. Technol. 86, 194–201 (2017).
[Crossref]

R. Ghorbani and F. M. Schmidt, “ICL-based TDLAS sensor for real-time breath gas analysis of carbon monoxide isotopes,” Opt. Express 25(11), 12743–12752 (2017).
[Crossref]

V. Ruzsányi and M. P. Kalapos, “Breath acetone as a potential marker in clinical practice,” J. Breath Res. 11(2), 024002 (2017).
[Crossref]

2016 (4)

R. D. Christensen, D. T. Malleske, D. K. Lambert, V. L. Baer, J. T. Prchal, L. E. Denson, E. Gerday, K. A. Weaver Lewis, and J. G. Shepherd, “Measuring end-tidal carbon monoxide of jaundiced neonates in the birth hospital to identify those with hemolysis,” Neonatology 109(1), 1–5 (2016).
[Crossref]

C. Jiang, M. Sun, Z. Wang, Z. Chen, X. Zhao, Y. Yuan, Y. Li, and C. Wang, “A portable Real-Time Ringdown Breath Acetone Analyzer: Toward Potential Diabetic Screening and Management,” Sensors 16(8), 1199 (2016).
[Crossref]

Z. H. Du, H. Gao, and X. H. Cao, “Direct high-precision measurement of the effective optical path length of multi-pass cell with optical frequency domain reflectometer,” Opt. Express 24(1), 417–426 (2016).
[Crossref]

Z. H. Du, G. Luo, Y. An, and J. Li, “Dynamic spectral characteristics measurement of DFB interband cascade laser under injection current tuning,” Appl. Phys. Lett. 109(1), 011903 (2016).
[Crossref]

2015 (4)

A. Reyes-Reyes, R. C. Horsten, and N. Bhattacharya, “Study of the exhaled acetone in type 1 diabetes using quantum cascade laser spectroscopy,” Anal. Chem. 87(1), 507–512 (2015).
[Crossref]

Y. N. Liu, J. Chang, J. Liu, Z. J. Liu, Q. Wang, and C. G. Zhu, “A time difference method for measurement of phase shift between distributed feedback laser diode (DFB-LD) output wavelength and intensity,” Sensors 15(7), 16153–16161 (2015).
[Crossref]

J. Li, Z. Du, and Y. An, “Frequency modulation characteristics for interband cascade lasers emitting at 3 μm,” Appl. Phys. B 121(1), 7–17 (2015).
[Crossref]

K. Liu, L. Wang, T. Tan, G. Wang, W. Zhang, W. Chen, and X. Gao, “Highly sensitive detection of methane by near-infrared laser absorption spectroscopy using a compact dense-pattern multipass cell,” Sens. Actuators B 220(1), 1000–1005 (2015).
[Crossref]

2014 (4)

L. Zuo, M. S. Koozechian, and L. L. Chen, “Characterization of reactive nitrogen species in allergic asthma,” Ann. Allergy, Asthma, Immunol. 112(1), 18–22 (2014).
[Crossref]

D. Smith, R. Spanel, J. Herbig, and J. Beauchamp, “Mass spectrometry for real-time quantitative breath analysis,” J. Breath Res. 8(2), 027101 (2014).
[Crossref]

C. D. Natale, R. Paolesse, E. Martinelli, and R. Capuano, “Solid-state gas sensors for breath analysis: A review,” Anal. Chim. Acta 824, 1–17 (2014).
[Crossref]

A. Amann, B. Costello, W. Miekisch, J. Schubert, B. Buszewski, J. Pleil, N. Ratcliffeand, and T. Risby, “The human volatilome: volatile organic compounds (VOCs) in exhaled breath, skin emanations, urine, feces and saliva,” J. Breath Res. 8(3), 034001 (2014).
[Crossref]

2013 (4)

K. Krzempek, M. Jahjah, R. Lewicki, P. Stefanski, S. So, D. Thomazy, and F. K. Tittel, “CW DFB RT diode laser-based sensor for trace-gas detection of ethane using a novel compact multipass gas absorption cell,” Appl. Phys. B. 112(4), 461–465 (2013).
[Crossref]

F. Zhu, H. Hundertmark, A. A. Kolomenskii, J. Strohaber, R. Holzwarth, and H. A. Schuessler, “High-power mid-infrared frequency comb source based on a femtosecond Er:fiber oscillator,” Opt. Lett. 38(13), 2360–2362 (2013).
[Crossref]

I. Galli, M. S. de Cumis, F. Cappelli, S. Bartalini, D. Mazzotti, S. Borri, A. Montori, N. Akikusa, M. Yamanishi, G. Giusfredi, P. Cancio, and P. De Natale, “Comb-assisted subkilohertz linewidth quantum cascade laser for high-precision mid-infrared spectroscopy,” Appl. Phys. Lett. 102(12), 121117 (2013).
[Crossref]

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
[Crossref]

2012 (3)

K. H. Kim, S. A. Jahan, and E. Kabir, “A review of breath analysis for diagnosis of human health,” Trends Anal. Chem. 33, 1–8 (2012).
[Crossref]

R. J. Basseri, B. Basseri, M. Pimentel, K. Chong, A. Youdim, K. Low, L. Hwang, E. Soffer, C. Chang, and R. Mathur, “Intestinal methane production in obese individuals is associated with a higher body mass index,” Gastroenterol. Hepatol. 8(1), 22–28 (2012).

F. G. Marcibdes-Braga, I. G. R. Gutz, G. L. Batista, P. H. Saldiva, S. M. Ayub-Ferreura, V. S. Issa, S. Mangini, E. A. Bocchi, and F. Bacal, “Exhaled acetone as a new biomarker of heart failure severity,” Chest 142(2), 457–466 (2012).
[Crossref]

2011 (1)

J. J. Harrison, N. D. C. Allen, and P. F. Bernath, “Infrared absorption cross sections for acetone (propanone) in the 3 um region,” J. Quant. Spectrosc. Radiat. Transfer 112(1), 53–58 (2011).
[Crossref]

2008 (2)

C. Wang and A. B. Surampudi, “An acetone breath analyzer using cavity ringdown spectroscopy: an initial test with human subjects under various situations,” Meas. Sci. Technol. 19(10), 105604 (2008).
[Crossref]

M. J. Thorpe, D. B. Clausen, M. S. Kirchner, and J. Ye, “Cavity-enhanced optical frequency comb spectroscopy: application to human breath analysis,” Opt. Express 16(4), 2387–2397 (2008).
[Crossref]

2006 (2)

J. Manne, O. Sukhorukov, W. Jäger, and J. Tulip, “Pulsed quantum cascade laser-based cavity ring-down spectroscopy for ammonia detection in breath,” Appl. Opt. 45(36), 9230–9237 (2006).
[Crossref]

W. Q. Cao and Y. X. Duan, “Breath analysis: potential for clinical diagnosis and exposure assessment,” Clin. Chem. 52(5), 800–811 (2006).
[Crossref]

2005 (1)

A. Lytkine, W. Jäger, and J. Tulip, “Long-wavelength VCSELs for applications in absorption spectroscopy: tuning rates and modulation performances,” Proc. SPIE 5737, 157–166 (2005).
[Crossref]

2004 (1)

W. Miekisch, J. K. Schubert, and G. Noeldge-Schomburg, “Diagnostic potential of breath analysis—focus on volatile organic compounds,” Clin. Chim. Acta 347(1-2), 25–39 (2004).
[Crossref]

2003 (1)

A. M. Diskin, P. Spanel, and D. Smith, “Time variation of ammonia, acetone, isoprene and ethanol in breath: a quantitative SIFT-MS study over 30 days,” Physiol Meas. 24(1), 107–119 (2003).
[Crossref]

2001 (2)

1993 (1)

1969 (1)

C. N. Tassopoulos, D. Barnett, and T. R. Fraser, “Breath-acetone and blood–sugar measurements in diabetes,” Lancet 293(7609), 1282–1286 (1969).
[Crossref]

Akikusa, N.

I. Galli, M. S. de Cumis, F. Cappelli, S. Bartalini, D. Mazzotti, S. Borri, A. Montori, N. Akikusa, M. Yamanishi, G. Giusfredi, P. Cancio, and P. De Natale, “Comb-assisted subkilohertz linewidth quantum cascade laser for high-precision mid-infrared spectroscopy,” Appl. Phys. Lett. 102(12), 121117 (2013).
[Crossref]

Allen, N. D. C.

J. J. Harrison, N. D. C. Allen, and P. F. Bernath, “Infrared absorption cross sections for acetone (propanone) in the 3 um region,” J. Quant. Spectrosc. Radiat. Transfer 112(1), 53–58 (2011).
[Crossref]

Aluauee, E.

A. Bicer, J. Bounds, F. Zhu, A. A. Kolomenski, N. Kaya, E. Aluauee, M. Amani, and H. A. Schuessler, “Sensitive Spectroscopic Analysis of Biomarkers in Exhaled Breath,” Int. J. Thermophys. 39(6), 69 (2018).
[Crossref]

Amani, M.

A. Bicer, J. Bounds, F. Zhu, A. A. Kolomenski, N. Kaya, E. Aluauee, M. Amani, and H. A. Schuessler, “Sensitive Spectroscopic Analysis of Biomarkers in Exhaled Breath,” Int. J. Thermophys. 39(6), 69 (2018).
[Crossref]

Amann, A.

A. Amann, B. Costello, W. Miekisch, J. Schubert, B. Buszewski, J. Pleil, N. Ratcliffeand, and T. Risby, “The human volatilome: volatile organic compounds (VOCs) in exhaled breath, skin emanations, urine, feces and saliva,” J. Breath Res. 8(3), 034001 (2014).
[Crossref]

An, Y.

Z. H. Du, G. Luo, Y. An, and J. Li, “Dynamic spectral characteristics measurement of DFB interband cascade laser under injection current tuning,” Appl. Phys. Lett. 109(1), 011903 (2016).
[Crossref]

J. Li, Z. Du, and Y. An, “Frequency modulation characteristics for interband cascade lasers emitting at 3 μm,” Appl. Phys. B 121(1), 7–17 (2015).
[Crossref]

Ayub-Ferreura, S. M.

F. G. Marcibdes-Braga, I. G. R. Gutz, G. L. Batista, P. H. Saldiva, S. M. Ayub-Ferreura, V. S. Issa, S. Mangini, E. A. Bocchi, and F. Bacal, “Exhaled acetone as a new biomarker of heart failure severity,” Chest 142(2), 457–466 (2012).
[Crossref]

Babikov, Y.

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
[Crossref]

Bacal, F.

F. G. Marcibdes-Braga, I. G. R. Gutz, G. L. Batista, P. H. Saldiva, S. M. Ayub-Ferreura, V. S. Issa, S. Mangini, E. A. Bocchi, and F. Bacal, “Exhaled acetone as a new biomarker of heart failure severity,” Chest 142(2), 457–466 (2012).
[Crossref]

Baer, V. L.

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I. Galli, M. S. de Cumis, F. Cappelli, S. Bartalini, D. Mazzotti, S. Borri, A. Montori, N. Akikusa, M. Yamanishi, G. Giusfredi, P. Cancio, and P. De Natale, “Comb-assisted subkilohertz linewidth quantum cascade laser for high-precision mid-infrared spectroscopy,” Appl. Phys. Lett. 102(12), 121117 (2013).
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J. Y. Li, G. Luo, Z. H. Du, and Y. W. Ma, “Hollow waveguide enhanced dimethyl sulfide sensor based on a 3.3 um interband cascade laser,” Sens. Actuators B 255, 3550–3557 (2018).
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C. D. Natale, R. Paolesse, E. Martinelli, and R. Capuano, “Solid-state gas sensors for breath analysis: A review,” Anal. Chim. Acta 824, 1–17 (2014).
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L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
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Noeldge-Schomburg, G.

W. Miekisch, J. K. Schubert, and G. Noeldge-Schomburg, “Diagnostic potential of breath analysis—focus on volatile organic compounds,” Clin. Chim. Acta 347(1-2), 25–39 (2004).
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Orphal, J.

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
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Paolesse, R.

C. D. Natale, R. Paolesse, E. Martinelli, and R. Capuano, “Solid-state gas sensors for breath analysis: A review,” Anal. Chim. Acta 824, 1–17 (2014).
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Perevalov, V.

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
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Perrin, A.

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
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Philippe, L. C.

Pimentel, M.

R. J. Basseri, B. Basseri, M. Pimentel, K. Chong, A. Youdim, K. Low, L. Hwang, E. Soffer, C. Chang, and R. Mathur, “Intestinal methane production in obese individuals is associated with a higher body mass index,” Gastroenterol. Hepatol. 8(1), 22–28 (2012).

Pleil, J.

A. Amann, B. Costello, W. Miekisch, J. Schubert, B. Buszewski, J. Pleil, N. Ratcliffeand, and T. Risby, “The human volatilome: volatile organic compounds (VOCs) in exhaled breath, skin emanations, urine, feces and saliva,” J. Breath Res. 8(3), 034001 (2014).
[Crossref]

Polovtseva, E. R.

L. S. Rothman, I. E. Gordon, Y. Babikov, A. Barbe, D. Chris Benner, P. F. Bernath, M. Birk, L. Bizzocchi, V. Boudon, L. R. Brown, A. Campargue, K. Chance, E. A. Cohen, L. H. Coudert, V. M. Devi, B. J. Drouin, A. Fayt, J. M. Flaud, R. R. Gamache, J. J. Harrison, J. M. Hartmann, C. Hill, J. T. Hodges, D. Jacquemart, A. Jolly, J. Lamouroux, R. J. Le Roy, G. Li, D. A. Long, O. M. Lyulin, C. J. Mackie, S. T. Massie, S. Mikhailenko, H. S. P. Mueller, O. V. Naumenko, A. V. Nikitin, J. Orphal, V. Perevalov, A. Perrin, E. R. Polovtseva, C. Richard, M. A. H. Smith, E. Starikova, K. Sung, S. Tashkun, J. Tennyson, G. C. Toon, V. G. Tyuterev, and G. Wagner, “HITRAN 2012 molecular spectroscopic database,” J. Quant. Spectrosc. Radiat. Transfer 130, 4–50 (2013).
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Figures (10)

Fig. 1.
Fig. 1. The schematic of the experimental setup. DFB-ICL: distributed feedback interband cascade laser, M: flat mirrors, BS: beam splitter, HWP: half wave plate, RL: red alignment laser, OPM: off-axis parabolic mirror, ML: mode matching lenses, OG: optical grating, VP: vacuum pump, VG: vacuum gauge, DAQ: data acquisition card, SA: spectrum analyzer. PD1,2: HgCdTe detectors. The inset at the top left shows the reflection spots on the two mirrors of the Herriot cell.
Fig. 2.
Fig. 2. Characteristics of the ICL laser: (a) Wavelength tuning curves with currents changing from 20 mA to 80 mA at three different temperatures (data from Nanoplus). The slope of this dependence is increasing with the current from 0.09 to 0.16 nm/mA. (b) The laser output (measured by the photodetector voltage) for different scan frequencies at 15°C. (c) The laser output at scan frequency 1 Hz for different temperatures.
Fig. 3.
Fig. 3. (a) The spectrum of the signal obtained as the result of beating between the MIR ICL laser and the frequency comb lines. (b) The measured spectral profile of the MID ICL laser line.
Fig. 4.
Fig. 4. The acetone spectrum in the wavelength interval from 1.5 μm to 10 μm from the PNNL database. The selected absorption band for the acetone detection is depicted in the inset: the strong absorption band is shown by the red line and the experimentally determined laser tuning dependence is shown by the black line (the limits of the tuning range are indicated by the two vertical dashed lines). The absorbances of CH4 and H2O for (concentration × optical path) of 2 ppm × m and 5% ×m, respectively, in the spectral range from 3.360 μm to the 3.372 μm are plotted in the inset (blue line is methane and green line is H2O.
Fig. 5.
Fig. 5. The peak of the acetone absorption band fitted by the pseudo-Voigt function; the graph at the bottom shows the residue, i.e. the difference between the acetone spectrum from the PNNL database and the fit function.
Fig. 6.
Fig. 6. The illustration to determining IM/FM phase shift: (a) The simulated sine signal with two absorption peaks on the positive and negative slopes of the current at the up- and down-sweeps. (b) The experimental peaks detected with a direct absorption spectroscopy at the positive and negative slopes of the current scan. (d) The phase shift variations for different modulation frequencies.
Fig. 7.
Fig. 7. (a) Two selected scanning intervals A and B for acetone detection. (b) The normalized 2f-signal dependent on the modulated current of the laser.
Fig. 8.
Fig. 8. The normalized 2f-signal amplitude versus wavelength measured for acetone in two spectral intervals A and B (see Fig. 7(a)). The blue dashed line shows the result of the calculation with Eqs. (6,7). The arrow indicates the wavelength for the maximum 2f-signal, coinciding with the peak of the absorption. The inset shows a portion of the measured the 2f-signal with experimental points.
Fig. 9.
Fig. 9. The measured 2f-signal at different concentrations of the calibration gas. It is well fitted by the linear dependence.
Fig. 10.
Fig. 10. Results of the sensor tests: (a) The results for a 25 minutes continuous data acquisition with a 200 ppm acetone concentration mixture. (b) The histogram of the measured data points. (c) The Allan deviation of the measured data, showing the detection limits of 0.58 ppm and 0.12 ppm with averaging times of 1 s and 60 s, respectively.

Equations (11)

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V p ( x ) = y 0 + A [ m × L ( x ) + ( 1 m ) × G ( x ) ] ,
L ( x ) = 2 π w 4 ( x x c ) 2 + w 2 , G ( x ) = 4 ln 2 π w exp 4 ln 2 w 2 ( x x c ) 2 ,
I ( t ) = I ¯ + I cos ( ω t ) ,
v ( t ) = v ¯ + v cos ( ω t + ψ ) .
S 2 f = G I ¯ 2 { [ H 2 + Δ I 2 I ¯ ( H 1 + H 3 ) cos ψ ] 2 + [ Δ I 2 I ¯ ( H 1 H 3 ) sin ψ ] 2 } 1 / 2 ,
H k ( v ¯ , v ) = P χ L S 2 π π π φ ( v ¯ + Δ ν cos θ ) cos k θ d θ ,
A 2 f = max ( S 2 f ) min ( S 2 f ) G I ¯ P S χ L .
S / N = A 2 f / δ ,
Δ t = 1 2 ( t 1 + t 2 2 t c )
ψ = 2 π f Δ t N , Δ t N = 1 2 N k = 1 N Δ t k ,
C = ( 4790.8   V 2 f 6.15629 )  ppm .

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