Abstract

We report enhanced emission and gain narrowing in Rhodamine 590 perchlorate dye in an aqueous suspension of polystyrene microspheres. A systematic experimental study of the threshold condition for and the gain narrowing of the stimulated emission over a wide range of dye concentrations and scatterer number densities showed several interesting features, even though the transport mean free path far exceeded the system size. The conventional diffusive-reactive approximation to radiative transfer in an inhomogeneously illuminated random amplifying medium, which is valid for a transport mean-free path much smaller than the system size, is clearly inapplicable here. We propose a new probabilistic approach for the present case of dense, random, weak scatterers involving the otherwise rare and ignorable sub-mean-free-path scatterings, now made effective by the high gain in the medium, which is consistent with experimentally observed features.

© 1997 Optical Society of America

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References

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  1. N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes, E. Sauvain, “Laser action in strongly scattering media,” Nature 368, 436–438 (1994).
    [Crossref]
  2. W. L. Sha, C. H. Liu, R. R. Alfano, “Spectral and temporal measurements of laser action of Rhodamine-640 dye in strongly scattering media,” Opt. Lett. 19, 1922–1924 (1994).
    [Crossref] [PubMed]
  3. R. M. Balachandran, N. M. Lawandy, “Interface reflection effects in photonic paint,” Opt. Lett. 20, 1271–1273 (1995).
    [Crossref] [PubMed]
  4. M. Siddique, R. R. Alfano, G. A. Berger, M. Kempe, A. Z. Genack, “Time-resolved studies of stimulated emission from colloidal dye solutions,” Opt. Lett. 21, 450–452 (1996).
    [Crossref] [PubMed]
  5. R. M. Balachandran, D. P. Pacheo, N. M. Lawandy, “Laser action in polymeric gain media containing scattering particles,” Appl. Opt. 35, 640–643 (1996).
    [Crossref] [PubMed]
  6. H. C. van de Hulst, Light Scattering by Small Particles (Dover, New York, 1981), pp. 121–128, 176–177.
  7. A. Ishimaru, Wave Propagation and Scattering in Random Media (Academic, New York, 1978), pp. 29 and 30.
  8. B. G. Huth, “Direct gain measurements of an organic dye amplifier,” Appl. Phys. Lett. 16, 185–188 (1970).
    [Crossref]
  9. V. S. Letokhov, “Generation of light by a scattering medium with negative resonance absorption,” Sov. Phys. JETP 26, 835–840 (1968).
  10. A. Y. Zyuzin, “Transmission fluctuations and spectral rigidity of lasing states in random amplifying media,” Phys. Rev. E 51, 5274–5278 (1995).
    [Crossref]
  11. P. Pradhan, N. Kumar, “Localization of light in coherently amplifying media,” Phys. Rev. B 50, 9644–9647 (1994).
    [Crossref]
  12. Z. Q. Zheng, “Light amplification and localization in randomly layered media with gain,” Phys. Rev. B 52, 7960–7964 (1995).
    [Crossref]
  13. C. W. J. Bennakker, J. C. J. Paasschens, P. W. Brouwer, “Probability of reflection by a random laser,” Phys. Rev. Lett. 76, 1368–1371 (1996).
    [Crossref]
  14. P. D. Kaplan, M. H. Kao, A. G. Yodh, D. J. Pine, “Geometric constraints for the design of diffusing-wave spectroscopy experiments,” Appl. Opt. 32, 3828–3836 (1993).
    [Crossref] [PubMed]

1996 (3)

1995 (3)

R. M. Balachandran, N. M. Lawandy, “Interface reflection effects in photonic paint,” Opt. Lett. 20, 1271–1273 (1995).
[Crossref] [PubMed]

Z. Q. Zheng, “Light amplification and localization in randomly layered media with gain,” Phys. Rev. B 52, 7960–7964 (1995).
[Crossref]

A. Y. Zyuzin, “Transmission fluctuations and spectral rigidity of lasing states in random amplifying media,” Phys. Rev. E 51, 5274–5278 (1995).
[Crossref]

1994 (3)

P. Pradhan, N. Kumar, “Localization of light in coherently amplifying media,” Phys. Rev. B 50, 9644–9647 (1994).
[Crossref]

N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes, E. Sauvain, “Laser action in strongly scattering media,” Nature 368, 436–438 (1994).
[Crossref]

W. L. Sha, C. H. Liu, R. R. Alfano, “Spectral and temporal measurements of laser action of Rhodamine-640 dye in strongly scattering media,” Opt. Lett. 19, 1922–1924 (1994).
[Crossref] [PubMed]

1993 (1)

1970 (1)

B. G. Huth, “Direct gain measurements of an organic dye amplifier,” Appl. Phys. Lett. 16, 185–188 (1970).
[Crossref]

1968 (1)

V. S. Letokhov, “Generation of light by a scattering medium with negative resonance absorption,” Sov. Phys. JETP 26, 835–840 (1968).

Alfano, R. R.

Balachandran, R. M.

Bennakker, C. W. J.

C. W. J. Bennakker, J. C. J. Paasschens, P. W. Brouwer, “Probability of reflection by a random laser,” Phys. Rev. Lett. 76, 1368–1371 (1996).
[Crossref]

Berger, G. A.

Brouwer, P. W.

C. W. J. Bennakker, J. C. J. Paasschens, P. W. Brouwer, “Probability of reflection by a random laser,” Phys. Rev. Lett. 76, 1368–1371 (1996).
[Crossref]

Genack, A. Z.

Gomes, A. S. L.

N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes, E. Sauvain, “Laser action in strongly scattering media,” Nature 368, 436–438 (1994).
[Crossref]

Huth, B. G.

B. G. Huth, “Direct gain measurements of an organic dye amplifier,” Appl. Phys. Lett. 16, 185–188 (1970).
[Crossref]

Ishimaru, A.

A. Ishimaru, Wave Propagation and Scattering in Random Media (Academic, New York, 1978), pp. 29 and 30.

Kao, M. H.

Kaplan, P. D.

Kempe, M.

Kumar, N.

P. Pradhan, N. Kumar, “Localization of light in coherently amplifying media,” Phys. Rev. B 50, 9644–9647 (1994).
[Crossref]

Lawandy, N. M.

Letokhov, V. S.

V. S. Letokhov, “Generation of light by a scattering medium with negative resonance absorption,” Sov. Phys. JETP 26, 835–840 (1968).

Liu, C. H.

Paasschens, J. C. J.

C. W. J. Bennakker, J. C. J. Paasschens, P. W. Brouwer, “Probability of reflection by a random laser,” Phys. Rev. Lett. 76, 1368–1371 (1996).
[Crossref]

Pacheo, D. P.

Pine, D. J.

Pradhan, P.

P. Pradhan, N. Kumar, “Localization of light in coherently amplifying media,” Phys. Rev. B 50, 9644–9647 (1994).
[Crossref]

Sauvain, E.

N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes, E. Sauvain, “Laser action in strongly scattering media,” Nature 368, 436–438 (1994).
[Crossref]

Sha, W. L.

Siddique, M.

van de Hulst, H. C.

H. C. van de Hulst, Light Scattering by Small Particles (Dover, New York, 1981), pp. 121–128, 176–177.

Yodh, A. G.

Zheng, Z. Q.

Z. Q. Zheng, “Light amplification and localization in randomly layered media with gain,” Phys. Rev. B 52, 7960–7964 (1995).
[Crossref]

Zyuzin, A. Y.

A. Y. Zyuzin, “Transmission fluctuations and spectral rigidity of lasing states in random amplifying media,” Phys. Rev. E 51, 5274–5278 (1995).
[Crossref]

Appl. Opt. (2)

Appl. Phys. Lett. (1)

B. G. Huth, “Direct gain measurements of an organic dye amplifier,” Appl. Phys. Lett. 16, 185–188 (1970).
[Crossref]

Nature (1)

N. M. Lawandy, R. M. Balachandran, A. S. L. Gomes, E. Sauvain, “Laser action in strongly scattering media,” Nature 368, 436–438 (1994).
[Crossref]

Opt. Lett. (3)

Phys. Rev. B (2)

P. Pradhan, N. Kumar, “Localization of light in coherently amplifying media,” Phys. Rev. B 50, 9644–9647 (1994).
[Crossref]

Z. Q. Zheng, “Light amplification and localization in randomly layered media with gain,” Phys. Rev. B 52, 7960–7964 (1995).
[Crossref]

Phys. Rev. E (1)

A. Y. Zyuzin, “Transmission fluctuations and spectral rigidity of lasing states in random amplifying media,” Phys. Rev. E 51, 5274–5278 (1995).
[Crossref]

Phys. Rev. Lett. (1)

C. W. J. Bennakker, J. C. J. Paasschens, P. W. Brouwer, “Probability of reflection by a random laser,” Phys. Rev. Lett. 76, 1368–1371 (1996).
[Crossref]

Sov. Phys. JETP (1)

V. S. Letokhov, “Generation of light by a scattering medium with negative resonance absorption,” Sov. Phys. JETP 26, 835–840 (1968).

Other (2)

H. C. van de Hulst, Light Scattering by Small Particles (Dover, New York, 1981), pp. 121–128, 176–177.

A. Ishimaru, Wave Propagation and Scattering in Random Media (Academic, New York, 1978), pp. 29 and 30.

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Figures (11)

Fig. 1
Fig. 1

Emission spectra from the center spot and the side spot for the pure dye, C = 5 × 10-4 M, at three different pump energies.

Fig. 2
Fig. 2

Emission spectra of the pure dye, C = 5 × 10-4 M, for various pump energies.

Fig. 3
Fig. 3

Emission spectra at a fixed pump energy of 2.25 mJ and C = 5 × 10-4 M for various scatterer densities n. The inset shows the variation in peak intensity at a fixed pump energy of 9 mJ as a function of scatterer density.

Fig. 4
Fig. 4

Peak intensity as a function of pump energy for various n at C = 5 × 10-4 M. The intensities for n = 1.24 × 1012 cm-3 have been scaled down by a factor of 10.

Fig. 5
Fig. 5

FWHM as a function of pump energy for various n for C = 5 × 10-4 M.

Fig. 6
Fig. 6

Emission spectra of pure dye, C = 5 × 10-3 M, for various pump energies.

Fig. 7
Fig. 7

FWHM as a function of pump energy for various n and C = 5 × 10-3 M. Filled squares refer to peak A and open circles to peak B of Fig. 6.

Fig. 8
Fig. 8

Peak intensity as a function of pump energy for peaks A and B for various n and C = 5 × 10-3 M. Note the scale factors.

Fig. 9
Fig. 9

Emission spectra for C = 5 × 10-3 M, n = 1.24 × 1012 cm-3 for various pump energies. Note changes in relative intensities of the two peaks.

Fig. 10
Fig. 10

Emission spectra of (curve a) pure dye, (curve b) n = 1.24 × 1012 cm-3 for C = 5 × 10-3 M and pump energy 13.5 mJ. Curve a has been scaled up by a factor of 500.

Fig. 11
Fig. 11

Emission spectra of (curve a) pure dye, (curve b) n = 1.24 × 1011 cm-3 for C = 2.5 × 10-2M and pump energy 13.5 mJ. Curve a has been scaled up by a factor of 10.

Equations (2)

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WL21-exp-Ll*expWlg1,
W2 expWlgLl*1.

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