Abstract

We describe a ‘wet mirror’ apparatus for cw cavity-enhanced absorption measurements with Bacteriochlorophyll a (BChla) in solution and show that it achieves the full sensitivity gain (≈ 2.3 × 104) afforded by the finesse (3.4 × 104) and loss distribution of our optical resonator. This result provides an important proof-of-principle demonstration for solution-phase cavity-enhanced spectroscopy; straightforward extrapolation to a system with state-of-the-art low-loss mirrors and shot-noise-limited performance indicates that single molecule sensitivity in liquids is within reach of current technology. With the probe laser locked to the cavity resonance, our instrument achieves a sensitivity ≈ 3.4 × 10-8/√Hz (for a sample of length 1.75 mm) with 100 kHz bandwidth and can reliably detect sub-nM concentrations of BChla with 1 ms integration time.

© 2006 Optical Society of America

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  1. R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
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    [CrossRef]
  6. L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
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    [CrossRef] [PubMed]
  9. S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
    [CrossRef]
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  12. F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
    [CrossRef]
  13. I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
    [CrossRef] [PubMed]
  14. M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
    [CrossRef] [PubMed]
  15. H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
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    [CrossRef] [PubMed]
  18. A. M. van Oijen, M. Ketelaars, J. K¨ohler, T. J. Aartsma and J. Schmidt, "Spectroscopy of Individual Light- Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band," Biophys. J. 78, 1570-1577 (2000).
    [CrossRef] [PubMed]
  19. H. A. Schuessler, S. H. Chen, Z. Rong, Z. C. Tang and E. C. Benck, "Cavity-enhanced photothermal spectroscopy: dynamics, sensitivity and spatial resolution," Appl. Opt. 31, 2669-2677 (1992).
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    [CrossRef]

2006

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

2005

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
[CrossRef]

2004

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
[CrossRef]

2003

A. J. Hallock, E. Berman and R. N. Zare, "Ultratrace Kinetic Measurements of the Reduction of Methylene Blue," J. Am. Chem. Soc. 125, 1158-1159 (2003).
[CrossRef] [PubMed]

2002

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

S. Xu, G. Sha and J. Xie, "Cavity ring-down spectroscopy in the liquid phase," Rev. Sci. Instrum. 73, 255-258 (2002).
[CrossRef]

2001

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

2000

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

A. M. van Oijen, M. Ketelaars, J. K¨ohler, T. J. Aartsma and J. Schmidt, "Spectroscopy of Individual Light- Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band," Biophys. J. 78, 1570-1577 (2000).
[CrossRef] [PubMed]

A. C. R. Pipino, "Monolithic folded resonator for evanescent wave cavity ringdown spectroscopy," Appl. Opt. 39, 1449-1453 (2000).
[CrossRef]

1999

H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
[CrossRef]

1998

1992

1981

C. K. N. Patel and A. C. Tam, "Pulsed optoacoustic spectroscopy of condensed matter," Rev. Mod. Phys. 53, 517-550 (1981).
[CrossRef]

1976

M. E. Long, R. L. Swofford and A. C. Albrecht, "Thermal Lens Technique — New Method of Absorption Spectroscopy," Science 191, 183-185 (1976).
[CrossRef] [PubMed]

Agirregabiria, M.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Albrecht, A. C.

M. E. Long, R. L. Swofford and A. C. Albrecht, "Thermal Lens Technique — New Method of Absorption Spectroscopy," Science 191, 183-185 (1976).
[CrossRef] [PubMed]

Ariese, F.

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

Bearman, G. H.

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Bechtel, K. L.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

Benck, E. C.

Berganzo, J.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Berman, E.

A. J. Hallock, E. Berman and R. N. Zare, "Ultratrace Kinetic Measurements of the Reduction of Methylene Blue," J. Am. Chem. Soc. 125, 1158-1159 (2003).
[CrossRef] [PubMed]

Black, E. D.

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
[CrossRef]

Blanco, F. J.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Calle, A.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Chen, S. H.

Connolly, J. S.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Dominguez, C.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Eichwurzel, I.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Elizalde, J.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Fiedler, S. E.

S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
[CrossRef]

Gooijer, C.

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

Grudinin, I. S.

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
[CrossRef]

Hall, J. L.

Hallock, A. J.

A. J. Hallock, E. Berman and R. N. Zare, "Ultratrace Kinetic Measurements of the Reduction of Methylene Blue," J. Am. Chem. Soc. 125, 1158-1159 (2003).
[CrossRef] [PubMed]

Hese, A.

S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
[CrossRef]

Hibara, A.

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

Ilchenko, V. S.

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Janzen, A. F.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Kachanov, A. A.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

Ketelaars, M.

A. M. van Oijen, M. Ketelaars, J. K¨ohler, T. J. Aartsma and J. Schmidt, "Spectroscopy of Individual Light- Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band," Biophys. J. 78, 1570-1577 (2000).
[CrossRef] [PubMed]

Kimble, H. J.

H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
[CrossRef]

G. Rempe, R. J. Thompson, H. J. Kimble and R. Lalezari, "Measurement of ultralow losses in an optical interferometer," Opt. Lett. 17, 363-365 (1992).
[CrossRef] [PubMed]

Kinrot, N.

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

Kitamori, T.

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

Kossokovski, D.

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Kunz, R. E.

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

Lalezari, R.

Lechuga, L. M.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Leupold, D.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Libbrecht, K. G.

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
[CrossRef]

Long, M. E.

M. E. Long, R. L. Swofford and A. C. Albrecht, "Thermal Lens Technique — New Method of Absorption Spectroscopy," Science 191, 183-185 (1976).
[CrossRef] [PubMed]

Ma, L.-S.

Mabuchi, H.

H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
[CrossRef]

Maleki, L.

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Mayora, K.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

Nadeau, J. L.

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Nathan, M.

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

Paldus, B. A.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

Patel, C. K. N.

C. K. N. Patel and A. C. Tam, "Pulsed optoacoustic spectroscopy of condensed matter," Rev. Mod. Phys. 53, 517-550 (1981).
[CrossRef]

Pipino, A. C. R.

Rao, S. R.

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
[CrossRef]

Rempe, G.

Rong, Z.

Ruth, A. A.

S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
[CrossRef]

Salomon, Y.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Samuel, E. B.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Sanders, S. S.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

Sawada, T.

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

Scheer, H.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Scherz, A.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Schuessler, H. A.

Sha, G.

S. Xu, G. Sha and J. Xie, "Cavity ring-down spectroscopy in the liquid phase," Rev. Sci. Instrum. 73, 255-258 (2002).
[CrossRef]

Stiel, H.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Swofford, R. L.

M. E. Long, R. L. Swofford and A. C. Albrecht, "Thermal Lens Technique — New Method of Absorption Spectroscopy," Science 191, 183-185 (1976).
[CrossRef] [PubMed]

Tam, A. C.

C. K. N. Patel and A. C. Tam, "Pulsed optoacoustic spectroscopy of condensed matter," Rev. Mod. Phys. 53, 517-550 (1981).
[CrossRef]

Tang, Z. C.

Teuchner, K.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Thompson, R. J.

Tokeshi, M.

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

Ubachs, W.

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

Uchida, M.

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

van der Sneppen, L.

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

van Oijen, A. M.

A. M. van Oijen, M. Ketelaars, J. K¨ohler, T. J. Aartsma and J. Schmidt, "Spectroscopy of Individual Light- Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band," Biophys. J. 78, 1570-1577 (2000).
[CrossRef] [PubMed]

Wiskerke, A.

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

Xie, J.

S. Xu, G. Sha and J. Xie, "Cavity ring-down spectroscopy in the liquid phase," Rev. Sci. Instrum. 73, 255-258 (2002).
[CrossRef]

Xu, S.

S. Xu, G. Sha and J. Xie, "Cavity ring-down spectroscopy in the liquid phase," Rev. Sci. Instrum. 73, 255-258 (2002).
[CrossRef]

Ye, J.

H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
[CrossRef]

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. N.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

A. J. Hallock, E. Berman and R. N. Zare, "Ultratrace Kinetic Measurements of the Reduction of Methylene Blue," J. Am. Chem. Soc. 125, 1158-1159 (2003).
[CrossRef] [PubMed]

Anal. Bioanal. Chem.

R. E. Kunz, "Optimizing integrated optical chips for label-free (bio)chemical sensing," Anal. Bioanal. Chem. 384, 180-190 (2006);N. Kinrot and M. Nathan, "Investigation of a Periodically-Segmented Waveguide Fabry- Pérot Interferometer for Use as a Chemical/Biosensor," J. Lightwave Technol. 24, 2139-2145 (2006).
[CrossRef]

Anal. Chem.

K. L. Bechtel, R. N. Zare, A. A. Kachanov, S. S. Sanders and B. A. Paldus, "Moving beyond Traditional UVVisible Absorption Detection: Cavity Ring-Down Spectroscopy for HPLC," Anal. Chem. 77, 1177-1182 (2005).
[CrossRef] [PubMed]

M. Tokeshi, M. Uchida, A. Hibara, T. Sawada and T. Kitamori, "Determination of Subyoctomole Amounts of NonfluorescentMolecules Using a Thermal LensMicroscope: Subsingle-Molecule Determination," Anal. Chem. 73, 2112-2116 (2001).
[CrossRef] [PubMed]

Anal. Chim. Acta

L. van der Sneppen, A. Wiskerke, F. Ariese, C. Gooijer and W. Ubachs, "Improving the sensitivity of HPLC absorption detection by cavity ring-down spectroscopy in a liquid-only cavity" Anal. Chim. Acta 558, 2-6 (2006).
[CrossRef]

Appl. Opt.

Appl. Phys. B

H. Mabuchi, J. Ye and H. J. Kimble, "Full observation of single-atom dynamics in cavity QED," Appl. Phys. B 68, 1095-1108 (1999).
[CrossRef]

Biophys. J.

A. M. van Oijen, M. Ketelaars, J. K¨ohler, T. J. Aartsma and J. Schmidt, "Spectroscopy of Individual Light- Harvesting 2 Complexes of Rhodopseudomonas acidophila: Diagonal Disorder, Intercomplex Heterogeneity, Spectral Diffusion, and Energy Transfer in the B800 Band," Biophys. J. 78, 1570-1577 (2000).
[CrossRef] [PubMed]

J. Am. Chem. Soc.

A. J. Hallock, E. Berman and R. N. Zare, "Ultratrace Kinetic Measurements of the Reduction of Methylene Blue," J. Am. Chem. Soc. 125, 1158-1159 (2003).
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J. Appl. Phys.

E. D. Black, I. S. Grudinin, S. R. Rao and K. G. Libbrecht, "Enhanced photothermal displacement spectroscopy for thin-film characterization using a Fabry-Perot resonator," J. Appl. Phys. 95, 7655-7659 (2004).
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J. Micromech. Microeng.

F. J. Blanco, M. Agirregabiria, J. Berganzo, K. Mayora, J. Elizalde, A. Calle, C. Dominguez and L. M. Lechuga, "Microfluidic-optical integrated CMOS compatible devicesfor label-free biochemical sensing," J. Micromech. Microeng. 16, 1006-1016 (2006).
[CrossRef]

J. Opt. Soc. Am. B

Opt. Lett.

Photochem. Photobiol.

I. Eichwurzel, H. Stiel, K. Teuchner, D. Leupold, H. Scheer, Y. Salomon and A. Scherz, "Photophysical Consequences of Coupling Bacteriochlorophyll a with Serine and its Resulting Solubility in Water," Photochem. Photobiol. 72, 204-209 (2000);J. S. Connolly, E. B. Samuel and A. F. Janzen, "Effects of solvent on the fluorescence properties of bacteriochlorophyll a," Photochem. Photobiol. 36, 565-574 (1982).
[CrossRef] [PubMed]

Proc. SPIE

J. L. Nadeau, V. S. Ilchenko, D. Kossokovski, G. H. Bearman and L. Maleki, "High-Q whispering-gallery mode sensor in liquids," Proc. SPIE 4629, 172-180 (2002).
[CrossRef]

Rev. Mod. Phys.

C. K. N. Patel and A. C. Tam, "Pulsed optoacoustic spectroscopy of condensed matter," Rev. Mod. Phys. 53, 517-550 (1981).
[CrossRef]

Rev. Sci. Instrum.

S. Xu, G. Sha and J. Xie, "Cavity ring-down spectroscopy in the liquid phase," Rev. Sci. Instrum. 73, 255-258 (2002).
[CrossRef]

S. E. Fiedler, A. Hese and A. A. Ruth, "Incoherent broad-band cavity-enhanced absorption spectorscopy of liquids," Rev. Sci. Instrum. 76, 023107 (2005).
[CrossRef]

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M. E. Long, R. L. Swofford and A. C. Albrecht, "Thermal Lens Technique — New Method of Absorption Spectroscopy," Science 191, 183-185 (1976).
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A. E. Siegman, Lasers (University Science Books, Sausalito, 1986).

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Figures (2)

Fig. 1.
Fig. 1.

Schematic diagram of the experimental setup. PBS: polarizing beam-splitter; NBPS: non-polarizing beam-splitter; λ/4: quarter-wave plate; HV: high voltage. See text for other designations.

Fig. 2.
Fig. 2.

Cavity-enhanced estimate (αl)ce≈ versus nominal BChla concentration (see text).

Equations (41)

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

P sp = P inc e δ
P sp + = P inc e δ e αl
( αl ) sp = In [ P sp ] In [ P sp + ] .
Δ ( αl ) sp = { ( αl ) sp P sp } Δ P sp + { ( αl ) sp P sp + } Δ P sp +
= Δ P sp P sp Δ P sp + P sp + .
P ce = P inc ( r 1 2 g rt ) 2 r 1 2 ( 1 g rt ) 2 , g rt = r 1 r 2 e δ / 2
P ce + = P inc ( r 1 2 g rt + ) 2 r 1 2 ( 1 g rt + ) 2 , g rt + = r 1 r 2 e δ / 2 e αl = g rt e αl
( αl ) ce = In [ 1 π 2 F 1 + π 2 F R ] + In [ Q + π 2 F R + Q π 2 F ] ,
R P ce P inc , R + P ce + P inc , Q 1 R + 1 R .
( αl ) ce = π F ( R + R 1 R + ) = π F ( P ce + P ce P inc P ce + ) .
P inc ε P inc , P ce P rfl ( 1 ε ) P inc , P ce + P rfl + ( 1 ε ) P inc ,
R P rfl ( 1 ε ) P inc ε P inc R ε , R + P rfl + ( 1 ε ) P inc ε P inc R + ε ,
( αl ) ce π F ( P rfl + ( 1 ε ) P inc P rfl ( 1 ε ) P inc ε P inc P rfl + ( 1 ε ) P inc ) ,
( αl ) ce P ce + = π 2 F P inc P ce P ce + ( P inc P ce + ) 2 ,
( αl ) ce P ce + Δ P ce + = π 2 F 1 R 1 R + R + 1 R + ( Δ P ce + P ce + ) .
( αl ) ce P ce + Δ P ce + = U ce 1 ( Δ P ce + P ce + ) .
G op U ce U sp = U ce = ( π 2 F 1 R 1 R + R + 1 R + ) 1 .
1 R 1 R + R + 1 R + < 2 ,
( αl ) ce P ce + Δ P ce + < π F ( Δ P ce + P ce + ) .
π 2 1 R 1 R + R + 1 R + π 2 R + 1 R + < 1 ,
( αl ) ce F Δ F = π F R R + 1 R + ( Δ F F ) ,
( αl ) ce P inc Δ P inc = π 2 F R R + 1 R + 1 1 R + ( Δ P inc P inc ) ,
( αl ) ce P ce Δ P ce = π 2 F R 1 R + ( Δ P ce P ce ) ,
( αl ) cav P tr + Δ P tr + = π 2 F 1 R ε 1 R + ε R + ε 1 R + ε ( Δ P tr + P tr + ( 1 ε ) P inc ) ,
Δ P ce + P ce + ( S / q ) P ce + τ ( S / q ) P ce + τ = 1 ( S / q ) P ce + τ ,
( αl ) ce P ce + Δ P ce + U ce 1 ( S / q ) P ce + τ .
Δ ( αl ) ce = ( ( αl ) ce P ce + ) Δ P ce + ( ( αl ) ce P ce + ) η P ce + ,
Δ ( αl ) sp = ( ( αl ) sp P sp + ) Δ P sp + ( ( αl ) sp P sp + ) η P sp + .
U th : ce = ( P ce + ( αl ) ce P ce + ) 1 = 1 l P ce + ( P ce + α ) P ce + ,
U th : sp = ( P sp + ( αl ) sp P sp + ) 1 = 1 l P sp + ( P sp + α ) P sp + .
P ce + = P inc ( r 1 2 g rt + ) 2 r 1 2 ( 1 g rt + ) 2 ,
P ce + α = 2 l P inc g rt + ( r 1 2 g rt + ) ( 1 r 1 2 ) r 1 2 ( 1 g rt+ ) 3 ,
( P ce + α ) P ce + = 2 l P ce + g rt + ( 1 r 1 2 ) ( 1 g rt + ) ( r 1 2 g rt + )
U th : ce = 2 g rt + ( 1 r 1 2 ) ( 1 g rt + ) ( r 1 2 g rt + ) .
G th U th : ce U th : sp = 2 g rt + ( 1 r 1 2 ) ( 1 g rt + ) ( r 1 2 g rt + ) ,
Δ ( αl ) th : ce U th : ce 1 ( S / q ) P ce + τ
2 ( 1 g rt ) ( r 1 2 g rt ) g rt ( 1 r 1 2 ) ( P ce τ ) / ( h ̅ ω ) .
L = 1 g rt 2 ( 1 r 1 2 ) + ( 1 r 2 2 ) + δ ,
L + = 1 g rt + 2 ( 1 r 1 2 ) + ( 1 r 2 2 ) + δ + 2 αl .
2 π F + 2 π F = 2 π ( Δ f + Δ f ) = 2 αl ,
( αl ) Δ f = π ( Δ f + Δ f ) .

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