Abstract

We present a ringdown absorption spectrometer based on a continuous-wave CO laser in the mid-infrared spectral region near λ=5μm. Using a linear ringdown cavity (length, 0.5 m) with R>=99.99% mirrors, we observed a noise-equivalent absorption coefficient of 7×1011cm1Hz12. This is 2 orders of magnitude improved compared with previous values. With this setup we studied the spectroscopic detection of carbonyl sulfide (here abbreviated OCS) traces in ambient air and in exhaled breath. We achieved a detection limit of 7 parts in 1012 (parts per trillion) OCS in ambient air, which is unprecedented and shows great promise for environmental and biomedical applications.

© 2005 Optical Society of America

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  1. G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  4. D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
    [CrossRef]
  5. G. von Basum, D. Halmer, P. Hering, M. Mürtz, S. Schiller, F. Müller, A. Popp, and F. Kühnemann, Opt. Lett. 29, 797 (2004).
    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef] [PubMed]
  8. S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
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    [CrossRef] [PubMed]
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    [CrossRef]
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2004 (3)

2003 (2)

C. Roller, A. A. Kosterev, F. K. Tittel, K. Uehara, C. Gmachl, and D. L. Sivco, Opt. Lett. 28, 2052 (2003).
[CrossRef] [PubMed]

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

2002 (1)

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

2001 (2)

A. A. Kosterev, A. L. Malinovsky, F. K. Tittel, C. Gmachl, F. Capasso, D. L. Sivco, J. N. Baillargeon, A. L. Hutchinson, and A. Y. Cho, Appl. Opt. 40, 5522 (2001).
[CrossRef]

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

2000 (2)

G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
[CrossRef]

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

1998 (1)

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

1997 (1)

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

1991 (1)

Albrecht, T.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Baillargeon, J. N.

Becker, P. B.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Berden, G.

G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
[CrossRef]

Bevington, P. R.

P. R. Bevington, Data Reduction and Error Analysis for the Physical Sciences (McGraw-Hill, 1969).

Bingemer, H.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Burdick, J. F.

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

Capasso, F.

Cho, A. Y.

Conte, J. V.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Cope, K. A.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Curl, R. F.

Dahnke, H.

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

Deckelmann, H.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Drummond, J. R.

Fox, J.

Fried, A.

Gmachl, C.

Halmer, D.

Harb, C. C.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Harris, J. S.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Henry, B.

Hering, P.

D. Halmer, G. von Basum, P. Hering, and M. Mürtz, Rev. Sci. Instrum. 75, 2187 (2004).
[CrossRef]

G. von Basum, D. Halmer, P. Hering, M. Mürtz, S. Schiller, F. Müller, A. Popp, and F. Kühnemann, Opt. Lett. 29, 797 (2004).
[CrossRef] [PubMed]

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

Hutchinson, A. L.

Jiang, L.

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

Jones, N.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Kachanov, A. A.

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

Kleine, D.

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

Kosterev, A. A.

Krieg, J.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Krishnan, J. A.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Kuang, Z.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Kühnemann, F.

Malinovsky, A. L.

McCurdy, M.

Meijer, G.

G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
[CrossRef]

Müller, F.

Mürtz, M.

G. von Basum, D. Halmer, P. Hering, M. Mürtz, S. Schiller, F. Müller, A. Popp, and F. Kühnemann, Opt. Lett. 29, 797 (2004).
[CrossRef] [PubMed]

D. Halmer, G. von Basum, P. Hering, and M. Mürtz, Rev. Sci. Instrum. 75, 2187 (2004).
[CrossRef]

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

Notholt, J.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Orens, J. B.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Paldus, B. A.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Peeters, R.

G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
[CrossRef]

Popp, A.

Rex, M.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Rinsland, C. P.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Risby, T. H.

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Roller, C.

Romanini, D.

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

Rosas, I.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Sadeghi, N.

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

Schiller, S.

Schrems, O.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Sehnert, S. S.

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

Sivco, D. L.

So, S.

Spence, T. G.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Stoeckel, F.

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

Studer, S. M.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Tittel, F. K.

Toon, G. C.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Uehara, K.

Urban, W.

D. Kleine, H. Dahnke, W. Urban, P. Hering, and M. Mürtz, Opt. Lett. 26, 1606 (2000).
[CrossRef]

von Basum, G.

Weidman, D.

Weinzierl, C.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Weller, R.

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Wilke, B.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Wysocki, G.

Xie, J.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Yang, S.

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Zare, R. N.

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

Appl. Opt. (3)

Biomarkers (1)

S. S. Sehnert, L. Jiang, J. F. Burdick, and T. H. Risby, Biomarkers 7, 174 (2002).
[CrossRef] [PubMed]

Chem. Phys. Lett. (1)

D. Romanini, A. A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
[CrossRef]

Int. Rev. Phys. Chem. (1)

G. Berden, R. Peeters, and G. Meijer, Int. Rev. Phys. Chem. 19, 565 (2000).
[CrossRef]

J. Appl. Phys. (1)

B. A. Paldus, C. C. Harb, T. G. Spence, B. Wilke, J. Xie, J. S. Harris, and R. N. Zare, J. Appl. Phys. 83, 3991 (1998).
[CrossRef]

J. Heart Lung Transplant (1)

S. M. Studer, J. B. Orens, I. Rosas, J. A. Krishnan, K. A. Cope, S. Yang, J. V. Conte, P. B. Becker, and T. H. Risby, J. Heart Lung Transplant 20, 1158–1166 (2001)
[CrossRef] [PubMed]

Opt. Lett. (3)

Rev. Sci. Instrum. (1)

D. Halmer, G. von Basum, P. Hering, and M. Mürtz, Rev. Sci. Instrum. 75, 2187 (2004).
[CrossRef]

Science (1)

J. Notholt, Z. Kuang, C. P. Rinsland, G. C. Toon, M. Rex, N. Jones, T. Albrecht, H. Deckelmann, J. Krieg, C. Weinzierl, H. Bingemer, R. Weller, and O. Schrems, Science 300, 307 (2003)
[CrossRef] [PubMed]

Other (2)

HITRAN2000 spectral database, http://www.hitran.com.

P. R. Bevington, Data Reduction and Error Analysis for the Physical Sciences (McGraw-Hill, 1969).

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Figures (6)

Fig. 1
Fig. 1

Schematic diagram of the experimental setup: EOM, electro-optic modulator; PZTs, piezoceramic transducers; ADC, analog-to-digital converter.

Fig. 2
Fig. 2

Schematic of the gas system. The sample gas flow can be adjusted by means of mass-flow controllers. The pressure is kept constant independently of the gas flow.

Fig. 3
Fig. 3

Empty cavity decay time versus time. For an observation time of 160 s the relative 1 σ uncertainty of the mean value is 5 × 10 6 , corresponding to a noise-equivalent absorption of 7 × 10 11 cm 1 Hz 1 2 .

Fig. 4
Fig. 4

Spectrum of an OCS mixture in grade 5 nitrogen near 2038.95 cm 1 . Filled circles, experimental data; solid curve, calculated data based on HITRAN2000 (OCS mixing ratio, 22.25 ppb; pressure, 40 hPa). Errors bars are smaller than the size of the circles.

Fig. 5
Fig. 5

Measured absorption versus OCS concentration. The noise-equivalent (NEQ) OCS concentration is 3 ppt Hz 1 2 .

Fig. 6
Fig. 6

(a) Observed spectrum of ambient air containing ( 570 ± 40 ) ppm of CO 2 and ( 463 ± 7 ) ppt of OCS. (b) Observed spectrum of exhaled breath containing ( 3.778 ± 0.004 ) % CO 2 and ( 438 ± 9 ) ppt of OCS. Darker solid curve, experimental data; lighter solid curves; fitted spectra; dotted curves, fitted CO 2 spectra; dashed curves, fitted OCS spectra.

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