Abstract

Broad-bandwidth, high-spectral-resolution optical detection of human breath has identified multiple important biomarkers correlated with specific diseases and metabolic processes. This optical-frequency-comb-based breath analysis system comes with excellent performance in all criteria: high detection sensitivity, ability to identify and distinguish a large number of analytes, and simultaneous, real-time information processing. We demonstrate a minimum detectable absorption of 8×10-10 cm-1, a spectral resolution of 800 MHz, and 200 nm of spectral coverage from 1.5 to 1.7 µm where strong and unique molecular fingerprints exist for many biomarkers. We present a series of breath measurements including stable isotope ratios of CO2, breath concentrations of CO, and the presence of trace concentrations of NH3 in high concentrations of H2O.

© 2008 Optical Society of America

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2007 (4)

D. Marinov, J. M. Rey, M. G. Muller, and M. W. Sigrist, "Spectroscopic investigation of methylated amines by a cavity-ringdown-based spectrometer," Appl. Opt. 46, 3981-3986 (2007).
[CrossRef] [PubMed]

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

M. J. Thorpe, D. D. Hudson, K. D. Moll, J. Lasri, and J. Ye, "Cavity-ringdown molecular spectroscopy based on an optical frequency comb at 1.45-1.65 µm," Opt. Lett. 32, 307-309 (2007).
[CrossRef] [PubMed]

S. A. Diddams, L. Hollberg, and V. Mbele, "Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb," Nature 445, 627-630 (2007).
[CrossRef] [PubMed]

2006 (8)

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

J. Manne, O. Sukhorukov, W. Jager, and J. Tulip, "Pulsed quantum cascade laser-based cavity ring-down spectroscopy for ammonia detection in breath," Appl. Opt. 45, 9230-9237 (2006).
[CrossRef] [PubMed]

T. H. Risby and S. F. Solga, "Current status of clinical breath analysis," Appl. Phys. B. 85, 421-426 (2006).
[CrossRef]

W. Q. Cao and Y. X. Duan, "Breath analysis: Potential for clinical diagnosis and exposure assessment," Clin. Chem. 52, 800-811 (2006).
[CrossRef] [PubMed]

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

E. H. Wahl, S. M. Tan, S. Koulikov, B. Kharlamov, C. R. Rella, E. R. Crosson, D. Biswell, and B. A. Paldus, "Ultra-sensitive ethylene post-harvest monitor based on cavity ring-down spectroscopy," Opt. Express 14, 1673-1684 (2006).
[CrossRef] [PubMed]

2005 (3)

L. S. Rothman, et al., "The HITRAN 2004 molecular spectroscopic database," J. Quant. Spectrosc. Radiat. Transfer 96, 139-204 (2005).
[CrossRef]

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

R. F. Machado, et al., "Detection of lung cancer by sensor array analyses of exhaled breath," Am. J. Respir. Crit. Care Med. 171, 1286-1291 (2005).
[CrossRef] [PubMed]

2004 (2)

2002 (3)

J. Cunnington and P. Hormbrey, "Breath analysis to detect recent exposure to carbon monoxide," Postgrad. Med. J. 78, 233-237 (2002).
[CrossRef] [PubMed]

T. Gherman and D. Romanini, "Mode-locked cavity-enhanced absorption spectroscopy," Opt. Express 10, 1033-1042 (2002).
[PubMed]

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

2001 (2)

1998 (1)

J. Ye, L. S. Ma, and J. L. Hall, "Ultrasensitive detections in atomic and molecular physics: demonstration in molecular overtone spectroscopy," J. Opt. Soc. Am. B. 15, 6-15 (1998).
[CrossRef]

1997 (3)

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

J. Poirson, F. Bretenaker, M. Vallet, and A. L. Floch, "Analytical and experimental study of ringing effects in a Fabry-Perot cavity. Application to the measurement of high finesses," J. Opt. Soc. Am. B 14, 2811-2817 (1997).
[CrossRef]

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

1993 (1)

L. Lundsberg-Nielsen, F. Hegelund, and F. M. Nicolaisen, "Analysis of the high-resolution of ammonia (14NH3) in the near-infrared region, 6400-6900 cm-1," J. Mol. Spectrosc. 162, 230-245 (1993).
[CrossRef]

1990 (1)

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Adler, F.

Baollargeon, J. N.

Biswell, D.

Bretenaker, F.

Cao, W. Q.

W. Q. Cao and Y. X. Duan, "Breath analysis: Potential for clinical diagnosis and exposure assessment," Clin. Chem. 52, 800-811 (2006).
[CrossRef] [PubMed]

Capasso, F.

Ceccarini, A.

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

Chilese, F. C.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Cho, A. Y.

Crosson, E. R.

E. H. Wahl, S. M. Tan, S. Koulikov, B. Kharlamov, C. R. Rella, E. R. Crosson, D. Biswell, and B. A. Paldus, "Ultra-sensitive ethylene post-harvest monitor based on cavity ring-down spectroscopy," Opt. Express 14, 1673-1684 (2006).
[CrossRef] [PubMed]

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Cunnington, J.

J. Cunnington and P. Hormbrey, "Breath analysis to detect recent exposure to carbon monoxide," Postgrad. Med. J. 78, 233-237 (2002).
[CrossRef] [PubMed]

Dahnke, H.

H. Dahnke, D. Kleine, P. Hering, and M. Mürtz, "Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy," Appl. Phys. B 72, 971-975 (2001).
[CrossRef]

De Natale, P.

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

Di Francesco, F.

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

Diddams, S. A.

S. A. Diddams, L. Hollberg, and V. Mbele, "Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb," Nature 445, 627-630 (2007).
[CrossRef] [PubMed]

Dill, S.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Duan, Y. X.

W. Q. Cao and Y. X. Duan, "Breath analysis: Potential for clinical diagnosis and exposure assessment," Clin. Chem. 52, 800-811 (2006).
[CrossRef] [PubMed]

Fitzpatrick, R.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Floch, A. L.

France, T.

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Fuoco, R.

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

Gagliardi, G.

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

Gherman, T.

Gibson, G.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Glasser, J.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Glogowski, S.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Gmachl, C.

Gooldy, M.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Grimble, G. K.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Hall, J. L.

J. Ye, L. S. Ma, and J. L. Hall, "Ultrasensitive detections in atomic and molecular physics: demonstration in molecular overtone spectroscopy," J. Opt. Soc. Am. B. 15, 6-15 (1998).
[CrossRef]

Haus, H. A.

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Hegelund, F.

L. Lundsberg-Nielsen, F. Hegelund, and F. M. Nicolaisen, "Analysis of the high-resolution of ammonia (14NH3) in the near-infrared region, 6400-6900 cm-1," J. Mol. Spectrosc. 162, 230-245 (1993).
[CrossRef]

Hering, P.

H. Dahnke, D. Kleine, P. Hering, and M. Mürtz, "Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy," Appl. Phys. B 72, 971-975 (2001).
[CrossRef]

Higbee, D. J.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Hollberg, L.

S. A. Diddams, L. Hollberg, and V. Mbele, "Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb," Nature 445, 627-630 (2007).
[CrossRef] [PubMed]

Hormbrey, P.

J. Cunnington and P. Hormbrey, "Breath analysis to detect recent exposure to carbon monoxide," Postgrad. Med. J. 78, 233-237 (2002).
[CrossRef] [PubMed]

Hudson, D. D.

Hutchinson, A. L.

Ippen, E. P.

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Jager, W.

Jones, D. J.

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Jones, R. J.

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

Kachanov, A. A.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Karalus, R. J.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Kharlamov, B.

Kleine, D.

H. Dahnke, D. Kleine, P. Hering, and M. Mürtz, "Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy," Appl. Phys. B 72, 971-975 (2001).
[CrossRef]

Kosterev, A. A.

Koulikov, S.

Lasri, J.

Leitenstorfer, A.

Longbottom, C.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Lundsberg-Nielsen, L.

L. Lundsberg-Nielsen, F. Hegelund, and F. M. Nicolaisen, "Analysis of the high-resolution of ammonia (14NH3) in the near-infrared region, 6400-6900 cm-1," J. Mol. Spectrosc. 162, 230-245 (1993).
[CrossRef]

Ma, L. S.

J. Ye, L. S. Ma, and J. L. Hall, "Ultrasensitive detections in atomic and molecular physics: demonstration in molecular overtone spectroscopy," J. Opt. Soc. Am. B. 15, 6-15 (1998).
[CrossRef]

Machado, R. F.

R. F. Machado, et al., "Detection of lung cancer by sensor array analyses of exhaled breath," Am. J. Respir. Crit. Care Med. 171, 1286-1291 (2005).
[CrossRef] [PubMed]

Maddaloni, P.

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

Malara, P.

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

Malinovsky, A. L.

Mangino, D. J.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Manne, J.

Marinov, D.

Mbele, V.

S. A. Diddams, L. Hollberg, and V. Mbele, "Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb," Nature 445, 627-630 (2007).
[CrossRef] [PubMed]

McMillan, L. C.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

McSwiggan, K.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Misiewicz, J. J.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Moll, K. D.

M. J. Thorpe, D. D. Hudson, K. D. Moll, J. Lasri, and J. Ye, "Cavity-ringdown molecular spectroscopy based on an optical frequency comb at 1.45-1.65 µm," Opt. Lett. 32, 307-309 (2007).
[CrossRef] [PubMed]

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

Monk, S. D.

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Muller, M. G.

Mürtz, M.

H. Dahnke, D. Kleine, P. Hering, and M. Mürtz, "Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy," Appl. Phys. B 72, 971-975 (2001).
[CrossRef]

Nelson, L. E.

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Nicolaisen, F. M.

L. Lundsberg-Nielsen, F. Hegelund, and F. M. Nicolaisen, "Analysis of the high-resolution of ammonia (14NH3) in the near-infrared region, 6400-6900 cm-1," J. Mol. Spectrosc. 162, 230-245 (1993).
[CrossRef]

O'Keefe, A.

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

Owano, T. G.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Padgett, M. J.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Paldus, B. A.

E. H. Wahl, S. M. Tan, S. Koulikov, B. Kharlamov, C. R. Rella, E. R. Crosson, D. Biswell, and B. A. Paldus, "Ultra-sensitive ethylene post-harvest monitor based on cavity ring-down spectroscopy," Opt. Express 14, 1673-1684 (2006).
[CrossRef] [PubMed]

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Pathak, K.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Patterson, C.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Paul, J. B.

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

Payne-James, J. J.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Poirson, J.

Provencal, R. A.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Rella, C. R.

Rennie, M. J.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Rey, J. M.

Ricci, K. N.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Richman, B. A.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Risby, T. H.

T. H. Risby and S. F. Solga, "Current status of clinical breath analysis," Appl. Phys. B. 85, 421-426 (2006).
[CrossRef]

Romanini, D.

Rothman, L. S.

L. S. Rothman, et al., "The HITRAN 2004 molecular spectroscopic database," J. Quant. Spectrosc. Radiat. Transfer 96, 139-204 (2005).
[CrossRef]

Safdi, B.

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

Saykally, R. J.

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

Scherer, J. J.

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

Scrimgeour, C. M.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Sigrist, M. W.

Sivco, D. L.

Skeldon, K. D.

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Solga, S. F.

T. H. Risby and S. F. Solga, "Current status of clinical breath analysis," Appl. Phys. B. 85, 421-426 (2006).
[CrossRef]

Spence, T. G.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Sukhorukov, O.

Tamura, K.

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Tan, S. M.

Tauser, F.

Thorpe, M. J.

M. J. Thorpe, D. D. Hudson, K. D. Moll, J. Lasri, and J. Ye, "Cavity-ringdown molecular spectroscopy based on an optical frequency comb at 1.45-1.65 µm," Opt. Lett. 32, 307-309 (2007).
[CrossRef] [PubMed]

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

Tittel, F. K.

Todd, M. W.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Trivella, M. G.

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

Tulip, J.

Vallet, M.

Wahl, E. H.

Weiner, A. M.

Wood, A. J.

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

Wood, T. D.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Wood, W. L.

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Wyse, C. A.

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Xiao, S.

Ye, J.

M. J. Thorpe, D. D. Hudson, K. D. Moll, J. Lasri, and J. Ye, "Cavity-ringdown molecular spectroscopy based on an optical frequency comb at 1.45-1.65 µm," Opt. Lett. 32, 307-309 (2007).
[CrossRef] [PubMed]

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

J. Ye, L. S. Ma, and J. L. Hall, "Ultrasensitive detections in atomic and molecular physics: demonstration in molecular overtone spectroscopy," J. Opt. Soc. Am. B. 15, 6-15 (1998).
[CrossRef]

Zare, R. A.

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Am. J. Respir. Crit. Care Med. (1)

R. F. Machado, et al., "Detection of lung cancer by sensor array analyses of exhaled breath," Am. J. Respir. Crit. Care Med. 171, 1286-1291 (2005).
[CrossRef] [PubMed]

Anal. Chem. (1)

E. R. Crosson, K. N. Ricci, B. A. Richman, F. C. Chilese, T. G. Owano, R. A. Provencal, M. W. Todd, J. Glasser, A. A. Kachanov, B. A. Paldus, T. G. Spence, and R. A. Zare, "Stable Isotope ratios using cavity ring-down spectroscopy: Determination of 13C/12C for carbon dioxide in human breath," Anal. Chem. 74, 2003-2007 (2002).
[CrossRef] [PubMed]

Appl. Opt. (3)

Appl. Phys. B (2)

H. Dahnke, D. Kleine, P. Hering, and M. Mürtz, "Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy," Appl. Phys. B 72, 971-975 (2001).
[CrossRef]

L. E. Nelson, D. J. Jones, K. Tamura, H. A. Haus, and E. P. Ippen, "Ultrashort-pulse fiber ring lasers," Appl. Phys. B 65, 277-294 (1997).
[CrossRef]

Appl. Phys. B. (1)

T. H. Risby and S. F. Solga, "Current status of clinical breath analysis," Appl. Phys. B. 85, 421-426 (2006).
[CrossRef]

Chem. Rev. (1)

J. J. Scherer, J. B. Paul, A. O'Keefe, and R. J. Saykally, "Cavity Ringdown Laser Absorption Spectroscopy - History, Development, and Application to pulsed molecular beams," Chem. Rev. 97, 25-51 (1997).
[CrossRef] [PubMed]

Clin. Chem. (1)

W. Q. Cao and Y. X. Duan, "Breath analysis: Potential for clinical diagnosis and exposure assessment," Clin. Chem. 52, 800-811 (2006).
[CrossRef] [PubMed]

Gut. (1)

S. Dill, J. J. Payne-James, J. J. Misiewicz, G. K. Grimble, K. McSwiggan, K. Pathak, A. J. Wood, C. M. Scrimgeour, and M. J. Rennie, "Evaluation of 13C-urea breath test in the detection of Heliobacter pylori and in monitoring the effect of tripotassium dicitratobismuthate in non-ulcer dyspepsia," Gut. 31, 1237-1241 (1990).
[CrossRef] [PubMed]

J. Mol. Spectrosc. (1)

L. Lundsberg-Nielsen, F. Hegelund, and F. M. Nicolaisen, "Analysis of the high-resolution of ammonia (14NH3) in the near-infrared region, 6400-6900 cm-1," J. Mol. Spectrosc. 162, 230-245 (1993).
[CrossRef]

J. Opt. Soc. Am. B (1)

J. Opt. Soc. Am. B. (1)

J. Ye, L. S. Ma, and J. L. Hall, "Ultrasensitive detections in atomic and molecular physics: demonstration in molecular overtone spectroscopy," J. Opt. Soc. Am. B. 15, 6-15 (1998).
[CrossRef]

J. Quant. Spectrosc. Radiat. Transfer (1)

L. S. Rothman, et al., "The HITRAN 2004 molecular spectroscopic database," J. Quant. Spectrosc. Radiat. Transfer 96, 139-204 (2005).
[CrossRef]

Meas. Sci. Technol. (1)

C. Patterson, L. C. McMillan, C. Longbottom, G. Gibson, M. J. Padgett, and K. D. Skeldon, "Portable optical spectroscopy for accurate analysis of ethane in exhaled breath," Meas. Sci. Technol. 18, 1459-1463 (2007).
[CrossRef]

Microchem. J. (1)

F. Di Francesco, R. Fuoco, M. G. Trivella, and A. Ceccarini, "Breath analysis: trends in techniques and clinical applications," Microchem. J. 79, 405-410 (2005).
[CrossRef]

Nature (1)

S. A. Diddams, L. Hollberg, and V. Mbele, "Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb," Nature 445, 627-630 (2007).
[CrossRef] [PubMed]

New J. Phys. (1)

P. Maddaloni, P. Malara, G. Gagliardi, and P. De Natale, "Mid-infrared fibre-based optical comb," New J. Phys. 8, 262-269 (2006).
[CrossRef]

Opt. Express (3)

Opt. Lett. (2)

Postgrad. Med. J. (1)

J. Cunnington and P. Hormbrey, "Breath analysis to detect recent exposure to carbon monoxide," Postgrad. Med. J. 78, 233-237 (2002).
[CrossRef] [PubMed]

Resp. Med. (1)

K. D. Skeldon, L. C. McMillan, C. A. Wyse, S. D. Monk, G. Gibson, C. Patterson, T. France, C. Longbottom, and M. J. Padgett, "Application of laser spectoscopy for measurement of exhaled ethane in patients with lung cancer," Respir. Med. 100, 300-306 (2006).
[CrossRef]

Science. (1)

M. J. Thorpe, K. D. Moll, R. J. Jones, B. Safdi, and J. Ye, "Broadband Cavity Ringdown Spectroscopy for Sensitive and Rapic Molecular Detection," Science. 311, 1595-1599 (2006).
[CrossRef] [PubMed]

Spectroscopy (1)

W. L. Wood, D. J. Higbee, M. Gooldy, S. Glogowski, R. Fitzpatrick, R. J. Karalus, T. D. Wood, and D. J. Mangino, "Analysis of volatile metabolites by Gas Chromatography-Mass Spectrometry," Spectroscopy 21, 20-25 (2006).

Other (4)

R. Polikar, R. Shinar, V. Honavar, L. Udpa, and M. D. Porter, "Detection and identification of odorants using an electronic nose," in Proceedings of IEEE 26th International Conference Acoustics, Speech and Signal Processing 5, 3137-3140 (2001).

K. K. Lehmann, et al., "High finesse optical resonator for cavity ring-down spectroscopy based upon Brewster's angle prism retroreflectors," U. S. Patent 5973864 (1999).

C. Gohle, B. Stein, A. Schliesser, T. Udem, and T. W. Hänsch, "Cavity enhanced Optical Vernier Spectroscopy, broad band, high resolution, high sensitivity," arXiv:0706.1582 (2007).

T. Okuno, M. Hirano, T. Nakanishi, and M. Onishi, "Highly-nonlinear optical fibers and their applications," SEI Tech. Rev. 62, 34-40 (2006). http://www.sei.co.jp/tr_e/pdf/info/62-06.pdf.

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Figures (7)

Fig. 1.
Fig. 1.

Schematic of the cavity-enhanced direct-frequency-comb spectrometer, along with the gas handling system for breath analysis.

Fig. 2.
Fig. 2.

(a) The spectrum generated by the mode-locked fiber laser from 1.5 to 1.6 µm (red) and the amplified, Raman shifted, spectrum from 1.6 to 1.7 µm (blue). (b) The measured reflectivity of the cavity mirrors as a function of wavelength. (c) The measured absorption spectrum of the air in our laboratory from 1.5 µm to 1.7 µm.

Fig. 3.
Fig. 3.

The absorption detection noise floor as a function of the number of pictures averaged. The camera dark count noise is also shown.

Fig. 4.
Fig. 4.

The software flow chart for generating a spectrum from a reference and an absorption image.

Fig. 5.
Fig. 5.

A breath spectrum between 1.622 µm and 1.638 µm. Several windows in this region contain spectroscopic features of three isotopes of CO2, with nearly equal absorption strengths. (a) and (b) Two zoomed-in spectral windows where line positions and intensities of relevant CO2 transitions are shown. Besides CO2 peaks, strong absorption features of H2O and CH4 are detected in (b). (c) The entire range over which this condition exists.

Fig. 6.
Fig. 6.

(a) The CO2 and CO absorption spectra of student 1 (smoker) and student 2 (non-smoker) in the 1.564 µm spectral region, along with line intensities from the Hitran spectral database. The smoker’s obvious increase in CO concentration is clearly detected. (b) The breath concentration of CO2 in parts per thousand (ppt) and CO in parts per million (ppm) as a function of time during which the test subject holds their breath prior to exhaling into the sample bag.

Fig. 7.
Fig. 7.

The absorption spectrum of lab air superimposed over the spectrum of 4.4 ppm of NH3. Hitran line intensities for H2O are included to identify the absorption features of the lab air spectrum. The dashed grey line represents the typical concentration of NH3 contained in the breath of a patient at final stages of renal failure.

Equations (2)

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E t E inc = n = 1 ( R 1 ) R n 1 e ( 2 n 1 ) α L 2 e i ϕ n ( t ) .
ϕ n ( t ) = 2 π ( 2 n 1 ) [ L ν ( t ) c ( n 1 ) β L 2 c 2 ] .

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