Abstract

In light of the recent discovery of methane on Mars and its possible biological origin, a strategy is described for making in situ measurements of methane and its isotopes on the surface of Mars by laser spectroscopy in the 3.3-μm wavelength region. An instrument of reasonable mass (~1 lb) and power (few watts) is capable of measuring mixing ratios down to 0.1 part per 109 by volume, a hundred times lower than recently reported observations. Making accurate measurements of 13CH4 and CH3D will be more difficult. For measuring 313C to 10‰ and δD to 50‰, sample preconcentration will be required to ~3 parts per 106 by volume for δ13C and to ~40 parts per 106 by volume for δD. This need would be mitigated by the discovery of larger local abundances of methane near the source regions.

© 2005 Optical Society of America

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2004 (2)

D. L. Valentine, A. Chidthaisong, A. Rice, W. S. Reeburgh, S. C. Tyler, “Carbon and isotope fractionation by moderately thermophilic methanogens,” Geochim. Cosmochim. Acta 68, 1571–1590 (2004).
[CrossRef]

C. R. Webster, G. J. Flesch, R. Haberle, J. Bauman, “Mars Laser Hygrometer,” Appl. Opt. 43, 4436–4445 (2004).
[CrossRef] [PubMed]

2003 (3)

L. S. Rothman, A. Barbe, D. C. Benner, L. R. Brown, C. Camy-Peyret, M. R. Carleer, K. Chance, C. Clerbaux, V. Dana, V. M. Devi, A. Fayt, J.-M. Flaud, R. R. Gamache, A. Goldman, D. Jacquemart, K. W. Jucks, W. J. Lafferty, J.-Y. Mandin, S. T. Massie, V. Nemtchinov, D. A. Newnham, A. Perrin, C. P. Rinsland, J. Schroeder, K. M. Smith, M. A. H. Smith, K. Tang, R. A. Toth, J. Vander Auwera, P. Varanasi, K. Yoshino, “The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001,” J. Quant. Spectrosc. Radiat. Transfer 82, 5–44 (2003).
[CrossRef]

C. R. Webster, A. J. Heymsfield, “Water isotope ratios D/H, 18O/16O, 17O/16O in and out of clouds map dehydration pathways,” Science 302, 1742–1745 (2003).
[CrossRef] [PubMed]

M. Lackner, G. Totschnig, F. Winter, M. Ortsiefer, M.-C. Amann, R. Shau, J. Rosskopf, “Demonstration of methane spectroscopy using a vertical cavity surface emitting laser at 1.68 μm with up to 5 MHz repetition rate,” Meas. Sci. Technol. 14, 101–106 (2003).
[CrossRef]

2002 (5)

M. Loewenstein, J. H. Jost, J. Grose, J. Eilers, D. Lynch, S. Jensen, J. Marmie, “Argus: a new instrument for the measurement of stratospheric dynamical tracers N2O and CH4,” Spectrochim. Acta Part A 58, 2329–2349 (2002).
[CrossRef]

E. C. Richard, K. K. Kelly, R. H. Winkler, R. Wilson, T. L. Thompson, R. J. McLaughlin, A. L. Schmeltekopf, A. F. Tuck, “A fast-response near-IR tunable diode laser absorption spectrometer for in situ measurements of CH4in the upper troposphere and lower stratosphere,” Appl. Phys. B. 75, 183–194 (2002).
[CrossRef]

J. B. McManus, M. S. Zahniser, D. D. Nelson, L. R. Williams, C. E. Kolb, “Infrared laser spectrometer with balanced absorption for measurement of isotropic ratios of carbon gases,” Spectrochim. Acta 58, 2465–2479 (2002).
[CrossRef]

C. Gmachl, A. Straub, R. Colombelli, F. Capasso, D. L. Sivco, A. M. Sergent, A. Y. Cho, “Single mode, tunable distributed-feedback and multiple wavelength quantum cascade lasers,” IEEE J. Quantum Electron. 38, 569–581 (2002).
[CrossRef]

M. Beck, D. Hofstetter, T. Aellen, J. Faist, U. Oesterle, M. Ilegems, E. Gini, H. Melchior, “Continuous wave operation of a mid-infrared semiconductor laser at room temperature,” Science 295, 301–305 (2002).
[CrossRef] [PubMed]

2001 (5)

R. D. May, S. F. Forouhar, D. Crisp, W. S. Woodward, D. A. Paige, A. Pathare, W. V. Boynton, “The MVACS tunable diode laser spectrometers,” J. Geophys. Res. 106, 17673–17682 (2001).
[CrossRef]

K. Uehara, K. Yamamoto, T. Kikugawa, N. Yoshida, “Isotope analysis of environmental substances by a new laser-spectroscopic method utilizing different pathlengths,” Sens. Actuators B 74, 173–178 (2001).
[CrossRef]

H. Dahnke, D. Kleine, W. Urban, P. Hering, M. Murtz, “Isotopic ratio measurements of methane in ambient air using mid-IR cavity leak-out spectroscopy,” App. Phys. B. 72, 121–125 (2001).
[CrossRef]

C. R. Webster, G. J. Flesch, D. C. Scott, J. Swanson, R. D. May, W. S. Woodward, C. Gmachl, F. Capasso, D. L. Sivco, J. N. Baillargeon, A. L. Hutchinson, A. Y. Cho, “Quantum-cascade laser measurements of stratospheric methane and nitrous oxide,” Appl. Opt. 40, 321–326 (2001).
[CrossRef]

D. Sumner, “Microbial influences on local carbon isotopic ratios and their preservation in carbonates,” Astrobiology 1, 57–70 (2001).
[CrossRef]

2000 (2)

P. Bergamaschi, M. Braunlich, T. Marik, C. A. M. Brenninkmeijer, “Measurements of the carbon and hydrogen isotopes of atmospheric methane at Izana, Tenerife: seasonal cycles and synoptic scale variations,” J. Geophys. Res. 105, 14531–14546 (2000).
[CrossRef]

G. Berden, R. Peeters, G. Meijer, “Cavity ring-down spectroscopy: experimental schemes and applications,” Int. Rev. Phys. Chem. 19, 565–607 (2000), and references therein.
[CrossRef]

1999 (2)

1998 (1)

P. Bergamaschi, C. A. M. Brenninkmeijer, M. Hahn, T. Rockmann, D. H. Scharffe, P. J. Crutzen, N. F. Elansky, I. B. Belikov, N. B. A. Trivett, D. E. J. Worthy, “Isotope analysis based on source identification for atmospheric CH4and CO sampled across Russia using the Trans-Siberian railroad,” J. Geophys. Res. 103, 8227–8235 (1998).
[CrossRef]

1997 (1)

1996 (1)

1995 (2)

1994 (1)

1993 (1)

J. E. Ehleringer, R. K. Monson, “Evolutionary and ecological aspects of photosynthetic pathway variations,” Annu. Rev. Ecol. Syst. 24, 411–413 (1993).
[CrossRef]

1992 (1)

C. R. Webster, R. D. May, “In situ stratospheric measurements of CH4, 13CH4, N2O and OC18O using the BLISS tunable diode laser spectrometer,” Geophys. Res. Lett. 19, 45–48 (1992).
[CrossRef]

1988 (2)

Y. L. Yung, R. R. Friedl, J. P. Pinto, K. D. Bayes, J.-S. Wen, “Kinetic isotopic fractionation and the origin of HDO and CH3D in the solar system,” Icarus 74, 121–132 (1988).
[CrossRef]

L. R. Brown, “Methane line parameters from 3700 to 4136 cm−1,” Appl. Opt. 27, 3275–3279 (1988).
[CrossRef] [PubMed]

1987 (1)

G. W. Sachse, G. F. Hill, L. O. Wade, M. G. Perry, “Fast-response, high-precision carbon monoxide sensor using a tunable diode laser absorption technique,” J. Geophys. Res. 92, 2071–2081 (1987).
[CrossRef]

1982 (1)

C. M. Stevens, F. E. Rust, “The carbon isotopic composition of atmospheric methane,” J. Geophys. Res. 87, 4879–4882 (1982).
[CrossRef]

1981 (1)

M. H. O’Leary, “Carbon isotope fractionation in plants,” Phytochemistry 20, 553–557 (1981).
[CrossRef]

1964 (1)

Aellen, T.

M. Beck, D. Hofstetter, T. Aellen, J. Faist, U. Oesterle, M. Ilegems, E. Gini, H. Melchior, “Continuous wave operation of a mid-infrared semiconductor laser at room temperature,” Science 295, 301–305 (2002).
[CrossRef] [PubMed]

Amann, M.-C.

M. Lackner, G. Totschnig, F. Winter, M. Ortsiefer, M.-C. Amann, R. Shau, J. Rosskopf, “Demonstration of methane spectroscopy using a vertical cavity surface emitting laser at 1.68 μm with up to 5 MHz repetition rate,” Meas. Sci. Technol. 14, 101–106 (2003).
[CrossRef]

Baer, D. S.

Baillargeon, J. N.

Bamford, D. J.

D. J. Bamford, M. Loewenstein, H. Jost, D. J. Cook, “Spectroscopic detection of methane using a portable room-temperature mid-IR laser source based on guided-wave difference-frequency generation,” in Diode Lasers and Applications in Atmospheric Sensing, A. Fried, ed., Proc. SPIE4817, 188–195 (2002).
[CrossRef]

Barbe, A.

L. S. Rothman, A. Barbe, D. C. Benner, L. R. Brown, C. Camy-Peyret, M. R. Carleer, K. Chance, C. Clerbaux, V. Dana, V. M. Devi, A. Fayt, J.-M. Flaud, R. R. Gamache, A. Goldman, D. Jacquemart, K. W. Jucks, W. J. Lafferty, J.-Y. Mandin, S. T. Massie, V. Nemtchinov, D. A. Newnham, A. Perrin, C. P. Rinsland, J. Schroeder, K. M. Smith, M. A. H. Smith, K. Tang, R. A. Toth, J. Vander Auwera, P. Varanasi, K. Yoshino, “The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001,” J. Quant. Spectrosc. Radiat. Transfer 82, 5–44 (2003).
[CrossRef]

Bauman, J.

Bayes, K. D.

Y. L. Yung, R. R. Friedl, J. P. Pinto, K. D. Bayes, J.-S. Wen, “Kinetic isotopic fractionation and the origin of HDO and CH3D in the solar system,” Icarus 74, 121–132 (1988).
[CrossRef]

Beck, M.

M. Beck, D. Hofstetter, T. Aellen, J. Faist, U. Oesterle, M. Ilegems, E. Gini, H. Melchior, “Continuous wave operation of a mid-infrared semiconductor laser at room temperature,” Science 295, 301–305 (2002).
[CrossRef] [PubMed]

Beimann, K.

H. P. Klein, N. H. Horowitz, K. Beimann, “The search for extant life on Mars,” in Mars, H. H. Kieffer, B. M. Jakowsky, C. Snyder, M. Matthews, eds. (University of Arizona, Tucson, Ariz., 1992), Chap. 34.

Belikov, I. B.

P. Bergamaschi, C. A. M. Brenninkmeijer, M. Hahn, T. Rockmann, D. H. Scharffe, P. J. Crutzen, N. F. Elansky, I. B. Belikov, N. B. A. Trivett, D. E. J. Worthy, “Isotope analysis based on source identification for atmospheric CH4and CO sampled across Russia using the Trans-Siberian railroad,” J. Geophys. Res. 103, 8227–8235 (1998).
[CrossRef]

Benner, D. C.

L. S. Rothman, A. Barbe, D. C. Benner, L. R. Brown, C. Camy-Peyret, M. R. Carleer, K. Chance, C. Clerbaux, V. Dana, V. M. Devi, A. Fayt, J.-M. Flaud, R. R. Gamache, A. Goldman, D. Jacquemart, K. W. Jucks, W. J. Lafferty, J.-Y. Mandin, S. T. Massie, V. Nemtchinov, D. A. Newnham, A. Perrin, C. P. Rinsland, J. Schroeder, K. M. Smith, M. A. H. Smith, K. Tang, R. A. Toth, J. Vander Auwera, P. Varanasi, K. Yoshino, “The HITRAN molecular spectroscopic database: edition of 2000 including updates through 2001,” J. Quant. Spectrosc. Radiat. Transfer 82, 5–44 (2003).
[CrossRef]

Berden, G.

G. Berden, R. Peeters, G. Meijer, “Cavity ring-down spectroscopy: experimental schemes and applications,” Int. Rev. Phys. Chem. 19, 565–607 (2000), and references therein.
[CrossRef]

Bergamaschi, P.

P. Bergamaschi, M. Braunlich, T. Marik, C. A. M. Brenninkmeijer, “Measurements of the carbon and hydrogen isotopes of atmospheric methane at Izana, Tenerife: seasonal cycles and synoptic scale variations,” J. Geophys. Res. 105, 14531–14546 (2000).
[CrossRef]

P. Bergamaschi, C. A. M. Brenninkmeijer, M. Hahn, T. Rockmann, D. H. Scharffe, P. J. Crutzen, N. F. Elansky, I. B. Belikov, N. B. A. Trivett, D. E. J. Worthy, “Isotope analysis based on source identification for atmospheric CH4and CO sampled across Russia using the Trans-Siberian railroad,” J. Geophys. Res. 103, 8227–8235 (1998).
[CrossRef]

P. Bergamaschi, M. Schupp, G. W. Harris, “High-precision, direct measurements of 13CH4/12CH4and 12CH3D/12CH4ratios in atmospheric methane sources by means of a long-path tunable diode laser absorption spectrometer,” Appl. Opt. 33, 7704–7716 (1994).
[CrossRef] [PubMed]

Bernard, B. R.

J. M. Brooks, W. R. Bryant, B. R. Bernard, N. R. Cameron, “The nature of gas hydrates on the Nigerian continental slope,” presented at the Annals of the New York Academy of Sciences Third International Conference on Gas Hydrates, Park City, Utah, 18–22 July 1999.

Boynton, W. V.

R. D. May, S. F. Forouhar, D. Crisp, W. S. Woodward, D. A. Paige, A. Pathare, W. V. Boynton, “The MVACS tunable diode laser spectrometers,” J. Geophys. Res. 106, 17673–17682 (2001).
[CrossRef]

Brasseur, G.

G. Brasseur, S. Solomon, Aeronomy of the Middle Atmosphere, 2nd ed. (Reidel, Dortrecht, The Netherlands, 1986).
[CrossRef]

Braunlich, M.

P. Bergamaschi, M. Braunlich, T. Marik, C. A. M. Brenninkmeijer, “Measurements of the carbon and hydrogen isotopes of atmospheric methane at Izana, Tenerife: seasonal cycles and synoptic scale variations,” J. Geophys. Res. 105, 14531–14546 (2000).
[CrossRef]

Brenninkmeijer, C. A. M.

P. Bergamaschi, M. Braunlich, T. Marik, C. A. M. Brenninkmeijer, “Measurements of the carbon and hydrogen isotopes of atmospheric methane at Izana, Tenerife: seasonal cycles and synoptic scale variations,” J. Geophys. Res. 105, 14531–14546 (2000).
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R. Yang, MicroDevices Laboratory, Jet Propulsion Laboratory, Pasadena, Calif.

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[CrossRef]

Meas. Sci. Technol. (1)

M. Lackner, G. Totschnig, F. Winter, M. Ortsiefer, M.-C. Amann, R. Shau, J. Rosskopf, “Demonstration of methane spectroscopy using a vertical cavity surface emitting laser at 1.68 μm with up to 5 MHz repetition rate,” Meas. Sci. Technol. 14, 101–106 (2003).
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Science (2)

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K. Uehara, K. Yamamoto, T. Kikugawa, N. Yoshida, “Isotope analysis of environmental substances by a new laser-spectroscopic method utilizing different pathlengths,” Sens. Actuators B 74, 173–178 (2001).
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J. B. McManus, M. S. Zahniser, D. D. Nelson, L. R. Williams, C. E. Kolb, “Infrared laser spectrometer with balanced absorption for measurement of isotropic ratios of carbon gases,” Spectrochim. Acta 58, 2465–2479 (2002).
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Other (17)

C. R. Webster, R. T. Menzies, E. D. Hinkley, “Infrared laser absorption: theory and applications,” Laser Remote Chemical Analysis, R. M. Measures, ed. (Wiley, New York, 1988), Chap. 3.

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Y. L. Yung, W. B. DeMore, Photochemistry of Planetary Atmospheres (Oxford U. Press, New York, 1999).

C. P. McKay, R. L. Mancinelli, C. R. Stoker, R. A. Wharton, “The possibility of life on Mars during a water-rich past,” in Mars, H. H. Kieffer, B. M. Jakowsky, C. Snyder, M. Matthews, eds. (University of Arizona, Tucson, Ariz., 1992), Chap. 35.

H. P. Klein, N. H. Horowitz, K. Beimann, “The search for extant life on Mars,” in Mars, H. H. Kieffer, B. M. Jakowsky, C. Snyder, M. Matthews, eds. (University of Arizona, Tucson, Ariz., 1992), Chap. 34.

K. Horikoshi, W. D. Grant, Extremophiles: Microbial Life in Extreme Environments (Wiley, New York, 1998).

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D. J. Bamford, M. Loewenstein, H. Jost, D. J. Cook, “Spectroscopic detection of methane using a portable room-temperature mid-IR laser source based on guided-wave difference-frequency generation,” in Diode Lasers and Applications in Atmospheric Sensing, A. Fried, ed., Proc. SPIE4817, 188–195 (2002).
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R. Yang, MicroDevices Laboratory, Jet Propulsion Laboratory, Pasadena, Calif.

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Figures (4)

Fig. 1
Fig. 1

Vibration–rotation line positions and intensities that make up the main absorption band regions, as provided by the HITRAN 2000 line listing.39

Fig. 2
Fig. 2

Comparison of line positions and strengths of 12CH3D, 13CH4, and 12CH4 lines of the υ3 bands, as calculated from the HITRAN 2000 line listings.39 Note that these are line strengths, not absorption intensities that will show relative differences depending on the temperature and pressure.

Fig. 3
Fig. 3

Calculation of the transmission spectrum of a sample of 10-ppbv 12CH4 for Mars surface conditions of 7-mbar pressure, 220 K temperature, a path length of 40 m, and a laser linewidth of 20 MHz.

Fig. 4
Fig. 4

Second-harmonic absorption spectrum recorded by the ALIAS instrument during a flight in 1999 (previously unpublished) through Earth’s stratosphere, showing strong line features of 12CH4 (lines A, B) with an excellent signal-to-noise ratio, and also weaker 13CH4 lines identified by arrows. The second 13CH4 line (line C) is also shown expanded by 100 in the y axis for clarity.

Tables (4)

Tables Icon

Table 1 Variation in Methane Isotope Ratios

Tables Icon

Table 2 Needed Methane Amounts for Required Precisions

Tables Icon

Table 3 Mass Estimate of Laser Spectrometer for Mars Methane

Tables Icon

Table 4 Data Rate Inventories for an Entire Spectral Scan and an Onboard Processed Scan

Equations (3)

Equations on this page are rendered with MathJax. Learn more.

δ 13 C = [ ( 13 C / 12 C ) sample / ( 13 C / 12 C ) standard - 1 ] × 1000
δ D = [ ( D / H ) sample / ( D / H ) standard - 1 ] × 1000 ,
δ D = { ( [ CH 3 D ] / 4 [ CH 4 ] ) / ( [ HDO ] / 2 [ H 2 O ] ) - 1 } × 1000 .

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