Abstract

We characterize, for the first time to our knowledge, the laser-induced backward fluorescence (retrofluorescence) spectra that result from energy-pooling collisions between Cs atoms near a dissipative thin Cs layer on a glass substrate. We resolve, experimentally and theoretically, the laser spectroscopic problem of energy-pooling processes related to the nature of the glass–metallic vapor interface. Our study focused on the integrated laser-induced retrofluorescence spectra for the 455.5-nm (72P3/2–62S1/2) and 852.2-nm (62P3/2–62S1/2) lines as a function of laser scanning through pumping resonance at the 852.2-nm line. We experimentally investigate the retrofluorescence from 420 to 930 nm, induced by a diode laser tuned either in the wings or in the center of the pumping resonance line. We present a detailed theoretical model of the retrofluorescence signal based on the radiative transfer equation, taking into account the evanescent wave of the excited atomic dipole strongly coupled with a dissipative surface. Based on theoretical and experimental results, we evaluate the effective nonradiative transfer rate Ā62P3/2→62S1/2sf for atoms in the excited 62P3/2 level located in the near-field region of the surface of the cell. Values extracted from the energy-pooling process analysis are equivalent to those found directly from the 852.2-nm resonance retrofluorescence line. We show that the effective energy-pooling coefficients k̃72P3/2 and k̃72P1/2 are approximately equal. The agreement between theory and experiment is remarkably good, considering the simplicity of the model.

© 2002 Optical Society of America

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  1. M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).
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  10. M. Zinkin, MFIT version 0.3 (1997), http://www.ill.fr/tas/matlab/.

2001 (3)

1997 (1)

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

1996 (1)

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

1992 (1)

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

1975 (1)

R. R. Chance, A. Prock, and R. Silbey, “Comments on the classical theory of energy transfer,” J. Chem. Phys. 62, 2245–2253 (1975).

1937 (1)

J. B. Taylor and I. Langmuir, “Vapour pressure of Caesium by the positive ion method,” Phys. Rev. 51, 753–760 (1937).

Allegrini, M.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Babin, F.

Bloch, D.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

Bordo, V. G.

V. G. Bordo, J. Loerke, L. Jozefowski, and H.-G. Rubahn, “Two-photon laser spectroscopy of the gas boundary layer in crossed evanescent and volume waves,” Phys. Rev. A 64, 012903/1–11 (2001).

Chance, R. R.

R. R. Chance, A. Prock, and R. Silbey, “Comments on the classical theory of energy transfer,” J. Chem. Phys. 62, 2245–2253 (1975).

Chevrollier, M.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

de Tomasi, F.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Ducloy, M.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

Fichet, M.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

Fioretti, A.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Gagné, J.-M.

Gagné, M.-C.

Huennekens, J.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Jabbour, Z. J.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Jozefowski, L.

V. G. Bordo, J. Loerke, L. Jozefowski, and H.-G. Rubahn, “Two-photon laser spectroscopy of the gas boundary layer in crossed evanescent and volume waves,” Phys. Rev. A 64, 012903/1–11 (2001).

Lai, H. M.

Langmuir, I.

J. B. Taylor and I. Langmuir, “Vapour pressure of Caesium by the positive ion method,” Phys. Rev. 51, 753–760 (1937).

Le Bris, K.

Loerke, J.

V. G. Bordo, J. Loerke, L. Jozefowski, and H.-G. Rubahn, “Two-photon laser spectroscopy of the gas boundary layer in crossed evanescent and volume waves,” Phys. Rev. A 64, 012903/1–11 (2001).

Milosevic, S.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Namiotka, R. K.

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Oria, M.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

Prock, A.

R. R. Chance, A. Prock, and R. Silbey, “Comments on the classical theory of energy transfer,” J. Chem. Phys. 62, 2245–2253 (1975).

Rahmat, G.

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

Rubahn, H.-G.

V. G. Bordo, J. Loerke, L. Jozefowski, and H.-G. Rubahn, “Two-photon laser spectroscopy of the gas boundary layer in crossed evanescent and volume waves,” Phys. Rev. A 64, 012903/1–11 (2001).

Silbey, R.

R. R. Chance, A. Prock, and R. Silbey, “Comments on the classical theory of energy transfer,” J. Chem. Phys. 62, 2245–2253 (1975).

Taylor, J. B.

J. B. Taylor and I. Langmuir, “Vapour pressure of Caesium by the positive ion method,” Phys. Rev. 51, 753–760 (1937).

Verkerk, P.

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Wu, Z.

Zhao, K.

J. Chem. Phys. (1)

R. R. Chance, A. Prock, and R. Silbey, “Comments on the classical theory of energy transfer,” J. Chem. Phys. 62, 2245–2253 (1975).

J. Opt. Soc. Am. B (2)

J. Phys. (Paris) II (1)

M. Chevrollier, M. Fichet, M. Oria, G. Rahmat, D. Bloch, and M. Ducloy, “High resolution selective reflection spectroscopy as a probe of long-range surface interaction: measurement of the surface van der Waals attraction exerted on excited Cs atoms,” J. Phys. (Paris) II 2, 631–657 (1992).

J. Phys. B (1)

F. de Tomasi, S. Milosevic, P. Verkerk, A. Fioretti, M. Allegrini, Z. J. Jabbour, and J. Huennekens, “Experimental study of caesium 6PJ+6PJ→7PJ+6S energy pooling collisions and modelling of the excited atom density in the presence of optical pumping and radiation trapping,” J. Phys. B 30, 4991–5008 (1997).

Phys. Rev. (1)

J. B. Taylor and I. Langmuir, “Vapour pressure of Caesium by the positive ion method,” Phys. Rev. 51, 753–760 (1937).

Phys. Rev. A (2)

V. G. Bordo, J. Loerke, L. Jozefowski, and H.-G. Rubahn, “Two-photon laser spectroscopy of the gas boundary layer in crossed evanescent and volume waves,” Phys. Rev. A 64, 012903/1–11 (2001).

Z. J. Jabbour, R. K. Namiotka, J. Huennekens, M. Allegrini, S. Milosevic, and F. de Tomasi, “Energy-pooling collisions in cesium: 6PJ+6PJ→6S+(nl=7P,  6D,  8S, 4F),” Phys. Rev. A 54, 1372–1384 (1996).

Other (2)

L. Krause, “Sensitized fluorescence and quenching,” The Excited State in Chemical Physics, J. W. McGowan, ed. (Wiley, New York, 1975), pp. 267–316.

M. Zinkin, MFIT version 0.3 (1997), http://www.ill.fr/tas/matlab/.

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