Abstract

The spectroscopic study of molecular ions is of great importance to a variety of fields, but is challenging as ions are typically produced in plasmas containing many orders of magnitude more neutral molecules than ions. The successful technique of velocity modulation permits discrimination between ion and neutral absorption signals and has allowed the study of scores of molecular ions in the past quarter century. However, this technique has long been considered to be inappropriate for use with cavity-enhanced techniques, owing to the directional nature of the velocity modulation. Here we report what we believe to be the first demonstration of cavity-enhanced velocity modulation spectroscopy, utilizing a 2f phase-sensitive demodulation scheme. This approach offers the promise of combining very high-sensitivity spectroscopic techniques with ion-neutral discrimination, which could extend the applicability of velocity modulation to intrinsically weak transitions and to ions that cannot be produced in high abundance. The use of a cavity also permits Lamb dip spectroscopy, which offers higher resolution and precision in frequency measurements and may be useful in measuring collisional rate coefficients.

© 2010 Optical Society of America

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  1. T. A. Dixon and R. C. Woods, Phys. Rev. Lett.  34, 61 (1975).
    [CrossRef]
  2. T. Oka, Phys. Rev. Lett.  45, 531 (1980).
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    [CrossRef]
  4. S. K. Stephenson and R. J. Saykally, Chem. Rev.  105, 3220 (2005).
    [CrossRef] [PubMed]
  5. J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
    [CrossRef]
  6. C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
    [CrossRef]
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    [CrossRef]
  8. S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  12. M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
    [CrossRef]

2009

C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
[CrossRef]

2008

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

2005

S. K. Stephenson and R. J. Saykally, Chem. Rev.  105, 3220 (2005).
[CrossRef] [PubMed]

2003

J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
[CrossRef]

1998

1992

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

1991

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

1983

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

F. Roux, F. Michaud, and J. Verges, J. Mol. Spectrosc.  97, 253 (1983).
[CrossRef]

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

1980

T. Oka, Phys. Rev. Lett.  45, 531 (1980).
[CrossRef]

1975

T. A. Dixon and R. C. Woods, Phys. Rev. Lett.  34, 61 (1975).
[CrossRef]

Begemann, M. H.

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

Bohle, W.

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

DiGangi, J. P.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

Dixon, T. A.

T. A. Dixon and R. C. Woods, Phys. Rev. Lett.  34, 61 (1975).
[CrossRef]

Drever, R. W. P.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Ferguson, D. W.

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

Ford, G. M.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Gottfried, J. L.

C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
[CrossRef]

J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
[CrossRef]

Gudeman, C. S.

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

Guelachvili, G.

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

Hall, J. L.

J. Ye, L. S. Ma, and J. L. Hall, J. Opt. Soc. Am. B  15, 6 (1998).
[CrossRef]

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Havenith, M.

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

Hough, J.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Kowalski, F. V.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Ma, L. S.

Martin, P. A.

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

McCall, B. J.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
[CrossRef]

Michaud, F.

F. Roux, F. Michaud, and J. Verges, J. Mol. Spectrosc.  97, 253 (1983).
[CrossRef]

Morong, C. P.

C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
[CrossRef]

Munley, A. J.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Negru, B.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

Oka, T.

C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
[CrossRef]

J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
[CrossRef]

T. Oka, Phys. Rev. Lett.  45, 531 (1980).
[CrossRef]

Pfaff, J.

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

Rao, K. N.

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

Roux, F.

F. Roux, F. Michaud, and J. Verges, J. Mol. Spectrosc.  97, 253 (1983).
[CrossRef]

Saykally, R. J.

S. K. Stephenson and R. J. Saykally, Chem. Rev.  105, 3220 (2005).
[CrossRef] [PubMed]

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

Schneider, M.

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

Stephenson, S. K.

S. K. Stephenson and R. J. Saykally, Chem. Rev.  105, 3220 (2005).
[CrossRef] [PubMed]

Tom, B. A.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

Urban, W.

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

Verges, J.

F. Roux, F. Michaud, and J. Verges, J. Mol. Spectrosc.  97, 253 (1983).
[CrossRef]

Ward, H.

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Wiczer, M. B.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

Widicus Weaver, S. L.

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

Woods, R. C.

T. A. Dixon and R. C. Woods, Phys. Rev. Lett.  34, 61 (1975).
[CrossRef]

Ye, J.

Appl. Phys. B

R. W. P. Drever, J. L. Hall, F. V. Kowalski, J. Hough, G. M. Ford, A. J. Munley, and H. Ward, Appl. Phys. B  31, 97 (1983).
[CrossRef]

Chem. Rev.

S. K. Stephenson and R. J. Saykally, Chem. Rev.  105, 3220 (2005).
[CrossRef] [PubMed]

J. Chem. Phys.

J. L. Gottfried, B. J. McCall, and T. Oka, J. Chem. Phys.  118, 10890 (2003).
[CrossRef]

J. Mol. Spectrosc.

C. P. Morong, J. L. Gottfried, and T. Oka, J. Mol. Spectrosc.  255, 13 (2009).
[CrossRef]

D. W. Ferguson, K. N. Rao, P. A. Martin, and G. Guelachvili, J. Mol. Spectrosc.  153, 599 (1992).
[CrossRef]

F. Roux, F. Michaud, and J. Verges, J. Mol. Spectrosc.  97, 253 (1983).
[CrossRef]

S. L. Widicus Weaver, M. B. Wiczer, B. Negru, J. P. DiGangi, B. A. Tom, and B. J. McCall, J. Mol. Spectrosc.  249, 14 (2008).
[CrossRef]

J. Opt. Soc. Am. B

Mol. Phys.

M. Havenith, M. Schneider, W. Bohle, and W. Urban, Mol. Phys.  72, 1149 (1991).
[CrossRef]

Phys. Rev. Lett.

T. A. Dixon and R. C. Woods, Phys. Rev. Lett.  34, 61 (1975).
[CrossRef]

T. Oka, Phys. Rev. Lett.  45, 531 (1980).
[CrossRef]

C. S. Gudeman, M. H. Begemann, J. Pfaff, and R. J. Saykally, Phys. Rev. Lett.  50, 727 (1983).
[CrossRef]

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Figures (3)

Fig. 1
Fig. 1

Experimental setup.

Fig. 2
Fig. 2

Spectral lines of, a, N 2 * and, b, N 2 + , recorded simultaneously by using two lock-in amplifiers with different phase settings.

Fig. 3
Fig. 3

Simulated time-dependence of the N 2 + absorption, a, at line center; b, at the zero-crossing; and, c, at the minimum, compared with, d, the electric field. Trace e, time-dependent concentration of N 2 * .

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