Abstract

We consider several highly sensitive techniques commonly used in detection of atomic and molecular absorptions. Their basic operating principles and corresponding performances are summarized and compared. We then present our latest results on the ultrasensitive detection of molecular overtone transitions to illustrate the principle and application of the cavity-enhanced frequency-modulation (FM) spectroscopy. An external cavity is used to enhance the molecular response to the light field, and an FM technique is applied for shot-noise-limited signal recovery. A perfect match between the FM sideband frequency and the cavity free spectral range makes the detection process insensitive to the laser-frequency noise relative to the cavity, and, at the same time, overcomes the cavity bandwidth limit. Working with a 1.064-μm Nd:YAG laser, we obtained sub-Doppler overtone resonances of C2HD, C2H2, and CO2 molecules. A detection sensitivity of 5×10-13 of integrated absorption (1×10-14/cm) over 1-s averaging time has been achieved.

© 1998 Optical Society of America

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  43. K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
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    [Crossref] [PubMed]
  50. L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

1997 (1)

J. Ye, L.-S. Ma, and J. L. Hall, “Ultra-stable optical frequency reference at 1.064 μm using a C2HD molecular overtone transition,” IEEE Trans. Instrum. Meas. 46, 178 (1997);J. Ye, “Ultrasensitive high resolution laser spectroscopy and its application to optical frequency standards,” Ph.D. dissertation (University of Colorado at Boulder, Boulder, Colorado, 1997).
[Crossref]

1996 (1)

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

1995 (4)

M. L. Eickhoff and J. L. Hall, “Optical frequency standard at 532 nm,” IEEE Trans. Instrum. Meas. 44, 155–158 (1995);P. Jungner, M. Eickhoff, S. Swartz, J. Ye, J. L. Hall, and S. Waltman, “Absolute frequency of the molecular iodine transition R(56) 32-0 near 532 nm,” IEEE Trans. Instrum. Meas. 44, 151 (1995).
[Crossref]

P. Werle, “Laser excess noise and interferometric effects in frequency-modulated diode-laser spectrometers,” Appl. Phys. B 60, 499–506 (1995).
[Crossref]

D. R. Hjelme, S. Neegård, and E. Vartdal, “Optical interference fringe reduction in frequency-modulation spectroscopy experiments,” Opt. Lett. 20, 1731–1733 (1995).
[Crossref]

D. Romanini and K. K. Lehmann, “Cavity ring-down overtone spectroscopy of HCN, H13CN, and HC15N,” J. Chem. Phys. 102, 633–642 (1995).
[Crossref]

1994 (4)

1992 (1)

1990 (3)

L. S. Ma, L. E. Ding, and Z. Y. Bi, “Doppler-free two-photon modulation transfer spectroscopy in sodium dimers,” Appl. Phys. B 51, 233–237 (1990).
[Crossref]

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

L.-S. Ma and J. L. Hall, “Optical heterodyne spectroscopy enhanced by an external optical cavity: toward improved working standards,” IEEE J. Quantum Electron. 26, 2006–2012 (1990).
[Crossref]

1989 (1)

1988 (1)

A. O’Keefe and D. A. G. Deacon, “Cavity ring-down optical spectrometer for absorption measurements using pulsed laser sources,” Rev. Sci. Instrum. 59, 2544–2551 (1988).
[Crossref]

1986 (2)

G. R. Janik, C. B. Carlisle, and T. F. Gallagher, “Two-tone frequency-modulation spectroscopy,” J. Opt. Soc. Am. B 3, 1070–1074 (1986).
[Crossref]

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

1985 (4)

1983 (1)

1982 (1)

1981 (5)

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

G. C. Bjorklund and M. D. Levenson, “Sub-Doppler frequency-modulation spectroscopy of I2,” Phys. Rev. A 24, 166–169 (1981).
[Crossref]

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. Altmann, R. Baumgart, and C. Weitkamp, “Two-mirror multipass absorption cell,” Appl. Opt. 20, 995–999 (1981).
[Crossref] [PubMed]

L. S. Rothman and L. D. G. Young, “Infrared energy levels and intensities of carbon dioxide. II,” J. Quantum Spectrosc. Radiat. Transf. 25, 505–524 (1981).
[Crossref]

1980 (3)

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

H. J. Kimble, “Calculated enhancement for intracavity spectroscopy with a single-mode laser,” IEEE J. Quantum Electron. QE-16, 455–461 (1980).
[Crossref]

G. C. Bjorklund, “Frequency-modulation spectroscopy: a new method for measuring weak absorptions and dispersions,” Opt. Lett. 5, 15–17 (1980).
[Crossref] [PubMed]

1979 (1)

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

1978 (1)

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

1976 (2)

C. E. Wieman and T. W. Hänsch, “Doppler-free laser polarization spectroscopy,” Phys. Rev. Lett. 36, 1170–1173 (1976);M. D. Levenson and G. L. Eesley, “Polarization selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19, 1–17 (1979).
[Crossref]

J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave fronts,” Appl. Phys. Lett. 29, 788–790 (1976).
[Crossref]

1975 (1)

1972 (1)

T. W. Hänsch, A. L. Schawlow, and P. E. Toschek, “Ultrasensitive response of a cw dye laser to selective extinction,” IEEE J. Quantum Electron. QE-8, 802–804 (1972).
[Crossref]

1971 (1)

1962 (1)

1961 (1)

H. Wahlquist, “Modulation broadening of unsaturated Lorentzian lines,” J. Chem. Phys. 35, 1708–1710 (1961).
[Crossref]

1951 (1)

B. Smaller, “Precise determination of the magnetic moment of the deuteron,” Phys. Rev. 83, 812–820 (1951);R. V. Pound, “Electronic frequency stabilization of microwave oscillators,” Rev. Sci. Instrum. 17, 490–505 (1946).
[Crossref] [PubMed]

Altmann, J.

Baer, T.

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

Baev, V. M.

V. M. Baev and P. E. Toschek, “Sensitivity limits of laser intracavity spectroscopy,” in Optical Methods in Atmospheric Chemistry, H. I. Schiff and U. Platt, eds., Proc. SPIE1715, 381–392 (1993).
[Crossref]

Baumgart, R.

Bergquist, J. C.

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

Bi, Z. Y.

L. S. Ma, L. E. Ding, and Z. Y. Bi, “Doppler-free two-photon modulation transfer spectroscopy in sodium dimers,” Appl. Phys. B 51, 233–237 (1990).
[Crossref]

Bialas, J.

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

Bjorklund, G. C.

Blatt, R.

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

Bollinger, J. J.

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

Bordé, C. J.

J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave fronts,” Appl. Phys. Lett. 29, 788–790 (1976).
[Crossref]

Brillet, A.

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

Bushaw, B. A.

Cannon, B. D.

Carlisle, C. B.

Cerez, P.

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

Davis, L. M.

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

de Angelis, M.

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

De Labachelerie, M.

M. De Labachelerie, K. Nakagawa, and M. Ohtsu, “Ultranarrow 13C2H2 saturated-absorption lines at 1.5 μm,” Opt. Lett. 19, 840–842 (1994).
[Crossref] [PubMed]

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

Deacon, D. A. G.

A. O’Keefe and D. A. G. Deacon, “Cavity ring-down optical spectrometer for absorption measurements using pulsed laser sources,” Rev. Sci. Instrum. 59, 2544–2551 (1988).
[Crossref]

Dehmelt, H.

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

Ding, L. E.

L. S. Ma, L. E. Ding, and Z. Y. Bi, “Doppler-free two-photon modulation transfer spectroscopy in sodium dimers,” Appl. Phys. B 51, 233–237 (1990).
[Crossref]

Dinneen, T.

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

Dubé, P.

L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

Eickhoff, M. L.

M. L. Eickhoff and J. L. Hall, “Optical frequency standard at 532 nm,” IEEE Trans. Instrum. Meas. 44, 155–158 (1995);P. Jungner, M. Eickhoff, S. Swartz, J. Ye, J. L. Hall, and S. Waltman, “Absolute frequency of the molecular iodine transition R(56) 32-0 near 532 nm,” IEEE Trans. Instrum. Meas. 44, 151 (1995).
[Crossref]

Fairbank, W. M.

Felder, R.

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

Field, R. W.

M. Jacobson and R. W. Field, MIT, Cambridge, Mass. 02139 (private communications, 1996).

Fritschel, P.

Gagliardi, G.

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

Gallagher, T. F.

Garmire, E.

Gehrtz, M.

Gianfrani, L.

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

Greiner, U. J.

Hall, J. L.

J. Ye, L.-S. Ma, and J. L. Hall, “Ultra-stable optical frequency reference at 1.064 μm using a C2HD molecular overtone transition,” IEEE Trans. Instrum. Meas. 46, 178 (1997);J. Ye, “Ultrasensitive high resolution laser spectroscopy and its application to optical frequency standards,” Ph.D. dissertation (University of Colorado at Boulder, Boulder, Colorado, 1997).
[Crossref]

M. L. Eickhoff and J. L. Hall, “Optical frequency standard at 532 nm,” IEEE Trans. Instrum. Meas. 44, 155–158 (1995);P. Jungner, M. Eickhoff, S. Swartz, J. Ye, J. L. Hall, and S. Waltman, “Absolute frequency of the molecular iodine transition R(56) 32-0 near 532 nm,” IEEE Trans. Instrum. Meas. 44, 151 (1995).
[Crossref]

L.-S. Ma and J. L. Hall, “Optical heterodyne spectroscopy enhanced by an external optical cavity: toward improved working standards,” IEEE J. Quantum Electron. 26, 2006–2012 (1990).
[Crossref]

N. C. Wong and J. L. Hall, “Servo control of amplitude modulation in FM spectroscopy: demonstration of shot-noise limited detection,” J. Opt. Soc. Am. B 2, 1527–1533 (1985).
[Crossref]

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave fronts,” Appl. Phys. Lett. 29, 788–790 (1976).
[Crossref]

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

Haller, K. L.

K. L. Haller and P. C. D. Hobbs, “Double beam laser absorption spectroscopy: shot noise-limited performance at baseband with a novel electronic noise canceller,” in Optical Methods for Ultrasensitive Detection and Analysis: Techniques and Applications, B. L. Fearey, ed., Proc. SPIE1435, 298–309 (1991).
[Crossref]

Hänsch, T. W.

C. E. Wieman and T. W. Hänsch, “Doppler-free laser polarization spectroscopy,” Phys. Rev. Lett. 36, 1170–1173 (1976);M. D. Levenson and G. L. Eesley, “Polarization selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19, 1–17 (1979).
[Crossref]

W. M. Fairbank, T. W. Hänsch, and A. L. Schawlow, “Absolute measurement of very low sodium-vapor densities using laser resonance fluorescence,” J. Opt. Soc. Am. 65, 199–204 (1975).
[Crossref]

T. W. Hänsch, A. L. Schawlow, and P. E. Toschek, “Ultrasensitive response of a cw dye laser to selective extinction,” IEEE J. Quantum Electron. QE-8, 802–804 (1972).
[Crossref]

Hemmati, H.

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

Hjelme, D. R.

Hobbs, P. C. D.

K. L. Haller and P. C. D. Hobbs, “Double beam laser absorption spectroscopy: shot noise-limited performance at baseband with a novel electronic noise canceller,” in Optical Methods for Ultrasensitive Detection and Analysis: Techniques and Applications, B. L. Fearey, ed., Proc. SPIE1435, 298–309 (1991).
[Crossref]

Hohenstatt, M.

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

Hollberg, L.

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

Houser, G. D.

Hurst, G. S.

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

Hurst, W. S.

Itano, W. M.

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

Jacobson, M.

M. Jacobson and R. W. Field, MIT, Cambridge, Mass. 02139 (private communications, 1996).

Janik, G. R.

Kastler, A.

Katsuda, T.

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

Keller, R. A.

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

Kimble, H. J.

H. J. Kimble, “Calculated enhancement for intracavity spectroscopy with a single-mode laser,” IEEE J. Quantum Electron. QE-16, 455–461 (1980).
[Crossref]

Klingerberg, H. H.

Kramer, S. D.

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

Lehmann, K. K.

D. Romanini and K. K. Lehmann, “Cavity ring-down overtone spectroscopy of HCN, H13CN, and HC15N,” J. Chem. Phys. 102, 633–642 (1995).
[Crossref]

Levenson, M. D.

Ma, L. S.

L. S. Ma, L. E. Ding, and Z. Y. Bi, “Doppler-free two-photon modulation transfer spectroscopy in sodium dimers,” Appl. Phys. B 51, 233–237 (1990).
[Crossref]

Ma, L.-S.

J. Ye, L.-S. Ma, and J. L. Hall, “Ultra-stable optical frequency reference at 1.064 μm using a C2HD molecular overtone transition,” IEEE Trans. Instrum. Meas. 46, 178 (1997);J. Ye, “Ultrasensitive high resolution laser spectroscopy and its application to optical frequency standards,” Ph.D. dissertation (University of Colorado at Boulder, Boulder, Colorado, 1997).
[Crossref]

L.-S. Ma and J. L. Hall, “Optical heterodyne spectroscopy enhanced by an external optical cavity: toward improved working standards,” IEEE J. Quantum Electron. 26, 2006–2012 (1990).
[Crossref]

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

Man-Pichot, C. N.

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

Nakagawa, K.

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

M. De Labachelerie, K. Nakagawa, and M. Ohtsu, “Ultranarrow 13C2H2 saturated-absorption lines at 1.5 μm,” Opt. Lett. 19, 840–842 (1994).
[Crossref] [PubMed]

Neegård, S.

Neuhauser, W.

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

O’Keefe, A.

A. O’Keefe and D. A. G. Deacon, “Cavity ring-down optical spectrometer for absorption measurements using pulsed laser sources,” Rev. Sci. Instrum. 59, 2544–2551 (1988).
[Crossref]

Ohtsu, M.

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

M. De Labachelerie, K. Nakagawa, and M. Ohtsu, “Ultranarrow 13C2H2 saturated-absorption lines at 1.5 μm,” Opt. Lett. 19, 840–842 (1994).
[Crossref] [PubMed]

Payne, M. G.

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

Riris, H.

Robinson, H. G.

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

Romanini, D.

D. Romanini and K. K. Lehmann, “Cavity ring-down overtone spectroscopy of HCN, H13CN, and HC15N,” J. Chem. Phys. 102, 633–642 (1995).
[Crossref]

Rosasco, G. J.

Rothman, L. S.

L. S. Rothman and L. D. G. Young, “Infrared energy levels and intensities of carbon dioxide. II,” J. Quantum Spectrosc. Radiat. Transf. 25, 505–524 (1981).
[Crossref]

Schawlow, A. L.

W. M. Fairbank, T. W. Hänsch, and A. L. Schawlow, “Absolute measurement of very low sodium-vapor densities using laser resonance fluorescence,” J. Opt. Soc. Am. 65, 199–204 (1975).
[Crossref]

T. W. Hänsch, A. L. Schawlow, and P. E. Toschek, “Ultrasensitive response of a cw dye laser to selective extinction,” IEEE J. Quantum Electron. QE-8, 802–804 (1972).
[Crossref]

Schellenberg, F. M.

Seitzinger, N. K.

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

Shelkovnikov, A. S.

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

Shera, E. B.

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

Shirley, J. H.

Smaller, B.

B. Smaller, “Precise determination of the magnetic moment of the deuteron,” Phys. Rev. 83, 812–820 (1951);R. V. Pound, “Electronic frequency stabilization of microwave oscillators,” Rev. Sci. Instrum. 17, 490–505 (1946).
[Crossref] [PubMed]

Smith, R. L.

Soper, S. A.

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

Tam, A. C.

W. Zapka, M. D. Levenson, F. M. Schellenberg, A. C. Tam, and G. C. Bjorklund, “Continuous-wave Doppler-free two-photon frequency-modulation spectroscopy in Rb vapor,” Opt. Lett. 8, 27–29 (1983).
[Crossref] [PubMed]

A. C. Tam, “Photothermal spectroscopy as a sensitive spectroscopic tool,” in Optical Methods for Ultrasensitive Detection and Analysis: Techniques and Applications, B. L. Fearey, ed. Proc. SPIE1435, 114–127 (1991).
[Crossref]

Tate, D. A.

Tino, G. M.

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

Toscheck, P.

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

Toschek, P. E.

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

T. W. Hänsch, A. L. Schawlow, and P. E. Toschek, “Ultrasensitive response of a cw dye laser to selective extinction,” IEEE J. Quantum Electron. QE-8, 802–804 (1972).
[Crossref]

V. M. Baev and P. E. Toschek, “Sensitivity limits of laser intracavity spectroscopy,” in Optical Methods in Atmospheric Chemistry, H. I. Schiff and U. Platt, eds., Proc. SPIE1715, 381–392 (1993).
[Crossref]

Vartdal, E.

Vogel, K.

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

Wahlquist, H.

H. Wahlquist, “Modulation broadening of unsaturated Lorentzian lines,” J. Chem. Phys. 35, 1708–1710 (1961).
[Crossref]

Wang, L.-G.

Warner, R. A.

Weiss, R.

Weitkamp, C.

Werle, P.

P. Werle, “Laser excess noise and interferometric effects in frequency-modulated diode-laser spectrometers,” Appl. Phys. B 60, 499–506 (1995).
[Crossref]

Whitaker, T. J.

Whittaker, E. A.

Wieman, C. E.

C. E. Wieman and T. W. Hänsch, “Doppler-free laser polarization spectroscopy,” Phys. Rev. Lett. 36, 1170–1173 (1976);M. D. Levenson and G. L. Eesley, “Polarization selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19, 1–17 (1979).
[Crossref]

Wineland, D. J.

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

Wong, N. C.

Ye, J.

J. Ye, L.-S. Ma, and J. L. Hall, “Ultra-stable optical frequency reference at 1.064 μm using a C2HD molecular overtone transition,” IEEE Trans. Instrum. Meas. 46, 178 (1997);J. Ye, “Ultrasensitive high resolution laser spectroscopy and its application to optical frequency standards,” Ph.D. dissertation (University of Colorado at Boulder, Boulder, Colorado, 1997).
[Crossref]

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

Young, J. P.

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

Young, L. D. G.

L. S. Rothman and L. D. G. Young, “Infrared energy levels and intensities of carbon dioxide. II,” J. Quantum Spectrosc. Radiat. Transf. 25, 505–524 (1981).
[Crossref]

Zapka, W.

Appl. Opt. (4)

Appl. Phys. B (2)

P. Werle, “Laser excess noise and interferometric effects in frequency-modulated diode-laser spectrometers,” Appl. Phys. B 60, 499–506 (1995).
[Crossref]

L. S. Ma, L. E. Ding, and Z. Y. Bi, “Doppler-free two-photon modulation transfer spectroscopy in sodium dimers,” Appl. Phys. B 51, 233–237 (1990).
[Crossref]

Appl. Phys. Lett. (2)

J. L. Hall, L. Hollberg, T. Baer, and H. G. Robinson, “Optical heterodyne saturation spectroscopy,” Appl. Phys. Lett. 39, 680–682 (1981);R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, “Laser phase and frequency stabilization using an optical resonator,” Appl. Phys. B 31, 97–105 (1983).
[Crossref]

J. L. Hall and C. J. Bordé, “Shift and broadening of saturated absorption resonances due to curvature of the laser wave fronts,” Appl. Phys. Lett. 29, 788–790 (1976).
[Crossref]

Chem. Phys. Lett. (1)

E. B. Shera, N. K. Seitzinger, L. M. Davis, R. A. Keller, and S. A. Soper, “Detection of single fluorescent molecules,” Chem. Phys. Lett. 174, 553–557 (1990).
[Crossref]

IEEE J. Quantum Electron. (3)

L.-S. Ma and J. L. Hall, “Optical heterodyne spectroscopy enhanced by an external optical cavity: toward improved working standards,” IEEE J. Quantum Electron. 26, 2006–2012 (1990).
[Crossref]

T. W. Hänsch, A. L. Schawlow, and P. E. Toschek, “Ultrasensitive response of a cw dye laser to selective extinction,” IEEE J. Quantum Electron. QE-8, 802–804 (1972).
[Crossref]

H. J. Kimble, “Calculated enhancement for intracavity spectroscopy with a single-mode laser,” IEEE J. Quantum Electron. QE-16, 455–461 (1980).
[Crossref]

IEEE Trans. Instrum. Meas. (3)

P. Cerez, A. Brillet, C. N. Man-Pichot, and R. Felder, “He–Ne lasers stabilized by saturated absorption in iodine at 612 nm,” IEEE Trans. Instrum. Meas. TIM-29, 352–354 (1980).
[Crossref]

M. L. Eickhoff and J. L. Hall, “Optical frequency standard at 532 nm,” IEEE Trans. Instrum. Meas. 44, 155–158 (1995);P. Jungner, M. Eickhoff, S. Swartz, J. Ye, J. L. Hall, and S. Waltman, “Absolute frequency of the molecular iodine transition R(56) 32-0 near 532 nm,” IEEE Trans. Instrum. Meas. 44, 151 (1995).
[Crossref]

J. Ye, L.-S. Ma, and J. L. Hall, “Ultra-stable optical frequency reference at 1.064 μm using a C2HD molecular overtone transition,” IEEE Trans. Instrum. Meas. 46, 178 (1997);J. Ye, “Ultrasensitive high resolution laser spectroscopy and its application to optical frequency standards,” Ph.D. dissertation (University of Colorado at Boulder, Boulder, Colorado, 1997).
[Crossref]

J. Chem. Phys. (2)

D. Romanini and K. K. Lehmann, “Cavity ring-down overtone spectroscopy of HCN, H13CN, and HC15N,” J. Chem. Phys. 102, 633–642 (1995).
[Crossref]

H. Wahlquist, “Modulation broadening of unsaturated Lorentzian lines,” J. Chem. Phys. 35, 1708–1710 (1961).
[Crossref]

J. Opt. Soc. Am. (2)

J. Opt. Soc. Am. B (6)

J. Phys. (France) Colloq. (1)

J. L. Hall, L. Hollberg, L.-S. Ma, T. Baer, and H. G. Robinson, “Progress toward phase-stable optical frequency standards,” J. Phys. (France) Colloq. 42, Suppl. 12, C8 59–71 (1981).

J. Quantum Spectrosc. Radiat. Transf. (1)

L. S. Rothman and L. D. G. Young, “Infrared energy levels and intensities of carbon dioxide. II,” J. Quantum Spectrosc. Radiat. Transf. 25, 505–524 (1981).
[Crossref]

Opt. Commun. (2)

J. Bialas, R. Blatt, W. Neuhauser, and P. E. Toschek, “Ultrasensitive detection of light absorption by few ions,” Opt. Commun. 59, 27–30 (1986).
[Crossref]

K. Nakagawa, T. Katsuda, A. S. Shelkovnikov, M. de Labachelerie, and M. Ohtsu, “Highly sensitive detection of molecular absorption using a high finesse optical cavity,” Opt. Commun. 107, 369–372 (1994).
[Crossref]

Opt. Lett. (6)

Phys. Rev. (1)

B. Smaller, “Precise determination of the magnetic moment of the deuteron,” Phys. Rev. 83, 812–820 (1951);R. V. Pound, “Electronic frequency stabilization of microwave oscillators,” Rev. Sci. Instrum. 17, 490–505 (1946).
[Crossref] [PubMed]

Phys. Rev. A (1)

G. C. Bjorklund and M. D. Levenson, “Sub-Doppler frequency-modulation spectroscopy of I2,” Phys. Rev. A 24, 166–169 (1981).
[Crossref]

Phys. Rev. Lett. (3)

C. E. Wieman and T. W. Hänsch, “Doppler-free laser polarization spectroscopy,” Phys. Rev. Lett. 36, 1170–1173 (1976);M. D. Levenson and G. L. Eesley, “Polarization selective optical heterodyne detection for dramatically improved sensitivity in laser spectroscopy,” Appl. Phys. 19, 1–17 (1979).
[Crossref]

W. Neuhauser, M. Hohenstatt, P. Toscheck, and H. Dehmelt, “Optical sideband cooling of visible atom cloud confined in parabolic well,” Phys. Rev. Lett. 41, 233–236 (1978).
[Crossref]

M. de Angelis, G. Gagliardi, L. Gianfrani, and G. M. Tino, “Test of the symmetrization postulate for spin-0 particles,” Phys. Rev. Lett. 76, 2840–2843 (1996);R. C. Hilborn and C. L. Yuca, “Spectroscopic test of the symmetrization postulate for spin-0 nuclei,” Phys. Rev. Lett. 76, 2844–2847 (1996).
[Crossref] [PubMed]

Rev. Mod. Phys. (1)

G. S. Hurst, M. G. Payne, S. D. Kramer, and J. P. Young, “Resonance ionization spectroscopy and one-atom detection,” Rev. Mod. Phys. 51, 767–819 (1979).
[Crossref]

Rev. Sci. Instrum. (1)

A. O’Keefe and D. A. G. Deacon, “Cavity ring-down optical spectrometer for absorption measurements using pulsed laser sources,” Rev. Sci. Instrum. 59, 2544–2551 (1988).
[Crossref]

Other (8)

K. L. Haller and P. C. D. Hobbs, “Double beam laser absorption spectroscopy: shot noise-limited performance at baseband with a novel electronic noise canceller,” in Optical Methods for Ultrasensitive Detection and Analysis: Techniques and Applications, B. L. Fearey, ed., Proc. SPIE1435, 298–309 (1991).
[Crossref]

D. J. Wineland, W. M. Itano, J. J. Bollinger, J. C. Bergquist, and H. Hemmati, “Spectroscopy of stored ions using fluorescence techniques,”, in Laser-Based Ultrasensitive Spectroscopy and Detection V, R. A. Keller, ed. Proc. SPIE426, 65–70 (1983).
[Crossref]

See, for example, Ultrasensitive Laser Spectroscopy, D. S. Kliger, ed. (Academic, New York, 1983).

A. C. Tam, “Photothermal spectroscopy as a sensitive spectroscopic tool,” in Optical Methods for Ultrasensitive Detection and Analysis: Techniques and Applications, B. L. Fearey, ed. Proc. SPIE1435, 114–127 (1991).
[Crossref]

V. M. Baev and P. E. Toschek, “Sensitivity limits of laser intracavity spectroscopy,” in Optical Methods in Atmospheric Chemistry, H. I. Schiff and U. Platt, eds., Proc. SPIE1715, 381–392 (1993).
[Crossref]

L.-S. Ma, J. Ye, P. Dubé, and J. L. Hall, “Ultrasensitive FM spectroscopy enhanced by a high finesse optical cavity: application to overtone transitions of C2H2 & C2HD,” J. Opt. Soc. Am. B (to be published).

M. Jacobson and R. W. Field, MIT, Cambridge, Mass. 02139 (private communications, 1996).

J. L. Hall, J. Ye, L.-S. Ma, K. Vogel, and T. Dinneen, “Optical frequency standards: progress and applications,” in Laser Spectroscopy XIII, Y. Z. Wang, ed. (World Scientific, Singapore, 1997).

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Figures (6)

Fig. 1
Fig. 1

Optical spectrum and the detection principle for NICE-OHMS.

Fig. 2
Fig. 2

General experimental schematic for the NICE-OHMS spectrometer.

Fig. 3
Fig. 3

Demonstration of the noise-immune property of NICE-OHMS. The C2HD (ν2+3ν3)P(5) resonance signal is recovered by both cavity-dither lock-in (DC) detection and the NICE-OHMS technique, under the experimental conditions of a tight laser/cavity lock (left column) and a substantially deteriorated lock (right column).

Fig. 4
Fig. 4

Sensitivity measurement of the NICE-OHMS technique. The upper graph shows the level of the saturated absorption, while the lower graph shows the corresponding S/N obtained via NICE-OHMS. The noise-equivalent detection sensitivities (normalized to 1-s time constant) are 3×10-11 for cavity-dither detection and 5.2×10-13 for NICE-OHMS.

Fig. 5
Fig. 5

Line-shape comparison among the resonances of (a) CO2, (b) C2HD, and (c) C2H2, under the same experimental conditions.

Fig. 6
Fig. 6

Pressure-dependent linewidth changes for both CO2 resonances. The negative-going peak has a zero-pressure extrapolated linewidth of 100 kHz, half the value of the transit time broadening. These aspects lead us to tentatively identify this feature as arising from two-photon absorption.

Equations (3)

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(αL)min=2eBηP01/2,
(αL)min=2eBηP01/2 2J0(β)J1(β),
(αL)min=π2×finesse 2eBηP01/2 2J0(β)J1(β).

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