Abstract

We present an experimental study of the input–output characteristics of an ultrashort pumped π-conjugated polymer in solution. By comparing the results for configurations with zero, one, and two mirrors around the polymer, we show that the physics is driven by amplified spontaneous emission and not by cooperative emission. This finding is substantiated by picosecond-time-scale measurements of the evolution of the emission of the polymer. For the two-mirror configuration a sharply defined threshold for laser oscillation is found; the output of the laser exhibits strong pulsations.

© 1999 Optical Society of America

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  1. D. Moses, Appl. Phys. Lett. 60, 3215 (1992).
    [CrossRef]
  2. H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
    [CrossRef]
  3. W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
    [CrossRef]
  4. N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
    [CrossRef]
  5. F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
    [CrossRef]
  6. A. E. Siegman, Lasers (University Science, Mill Valley, Calif., 1986).
  7. A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
    [CrossRef]
  8. S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
    [CrossRef]
  9. S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
    [CrossRef]
  10. X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).
  11. H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
  12. H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
    [CrossRef]
  13. M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
    [CrossRef]
  14. J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
    [CrossRef]

1998 (3)

A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
[CrossRef]

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

1997 (4)

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

1996 (2)

N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
[CrossRef]

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

1995 (1)

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

1992 (1)

D. Moses, Appl. Phys. Lett. 60, 3215 (1992).
[CrossRef]

1988 (1)

J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
[CrossRef]

1981 (1)

M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
[CrossRef]

Andersson, M. R.

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Becker, H.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

Blau, W. J.

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Bor, Z.

J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
[CrossRef]

Bradley, D. D. C.

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Brouwer, H. J.

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Davey, A.

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Demandt, R.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

Denton, G. J.

N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
[CrossRef]

Diaz-Garcia, M. A.

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Dogariu, A.

A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
[CrossRef]

Friend, R. H.

N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
[CrossRef]

Frolov, S. V.

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

Gellermann, W.

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

Gong, S. H.

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Hadziioannou, G.

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Heeger, A. J.

A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
[CrossRef]

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Hide, F.

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Hilberer, A.

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Holzer, W.

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Inbasekaran, M.

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Klebniczki, J.

J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
[CrossRef]

Kluge, E.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

Krasnikov, V. V.

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Kreuder, H. S. W.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

Lane, P. A.

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

Liess, M.

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

Long, X.

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Malinowski, A.

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Moses, D.

D. Moses, Appl. Phys. Lett. 60, 3215 (1992).
[CrossRef]

Ozaki, M.

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

Pei, Q.

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Penzkofer, A.

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Polder, D.

M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
[CrossRef]

Schoo, H. F. M.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

Schuurmans, M. F. H.

M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
[CrossRef]

Schwartz, B. J.

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Siegman, A. E.

A. E. Siegman, Lasers (University Science, Mill Valley, Calif., 1986).

Spreitzer, H.

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

Szabó, G.

J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
[CrossRef]

Tessler, N.

N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
[CrossRef]

Vacar, D.

A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
[CrossRef]

Vardeny, Z. V.

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

Vrehen, Q. H. F.

M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
[CrossRef]

Wildeman, J.

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Woo, E. P.

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Yoshino, K.

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

Adv. Atom. Mol. Phys. (1)

M. F. H. Schuurmans, Q. H. F. Vrehen, and D. Polder, Adv. Atom. Mol. Phys. 17, 167 (1981).
[CrossRef]

Adv. Mater. (2)

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).

H. Spreitzer, H. Becker, E. Kluge, H. S. W. Kreuder, R. Demandt, and H. F. M. Schoo, Adv. Mater. 10, 1340 (1998).
[CrossRef]

Appl. Phys. B (1)

J. Klebniczki, Z. Bor, and G. Szabó, Appl. Phys. B 46, 151 (1988).
[CrossRef]

Appl. Phys. Lett. (2)

D. Moses, Appl. Phys. Lett. 60, 3215 (1992).
[CrossRef]

H. J. Brouwer, V. V. Krasnikov, A. Hilberer, J. Wildeman, and G. Hadziioannou, Appl. Phys. Lett. 66, 3404 (1995).
[CrossRef]

Chem. Phys. Lett. (1)

X. Long, A. Malinowski, D. D. C. Bradley, M. Inbasekaran, and E. P. Woo, Chem. Phys. Lett. 272, 6 (1997).

Nature (1)

N. Tessler, G. J. Denton, and R. H. Friend, Nature 382, 695 (1996).
[CrossRef]

Opt. Quantum Electron. (1)

W. Holzer, A. Penzkofer, S. H. Gong, A. Davey, and W. J. Blau, Opt. Quantum Electron. 29, 713 (1997).
[CrossRef]

Phys. Rev. B (1)

A. Dogariu, D. Vacar, and A. J. Heeger, Phys. Rev. B 58, 10218 (1998).
[CrossRef]

Phys. Rev. Lett. (2)

S. V. Frolov, M. Liess, P. A. Lane, W. Gellermann, and Z. V. Vardeny, Phys. Rev. Lett. 78, 4285 (1997).
[CrossRef]

S. V. Frolov, W. Gellermann, M. Ozaki, K. Yoshino, and Z. V. Vardeny, Phys. Rev. Lett. 78, 729 (1997).
[CrossRef]

Science (1)

F. Hide, M. A. Diaz-Garcia, B. J. Schwartz, M. R. Andersson, Q. Pei, and A. J. Heeger, Science 273, 1833 (1996).
[CrossRef]

Other (1)

A. E. Siegman, Lasers (University Science, Mill Valley, Calif., 1986).

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Figures (5)

Fig. 1
Fig. 1

Schematic of the experimental setup: The shaded area represents the dye cell, with the excitation region indicated by the oval. The laser cavity is formed by a concave high reflector (HR), R=-50 mm, and a flat output coupler (OC). To avoid optical feedback from the walls of the dye cell we tilt the latter slightly.

Fig. 2
Fig. 2

Light output versus pump energy for the (a) mirrorless, (b) single-mirror, and (c) full-cavity setup. Note the quantitative differences of the signal for the three configurations.

Fig. 3
Fig. 3

Temporal evolution of the light output for the single-pass setup when it is pumped with an ultrashort excitation pulse. The time axis is normalized to the spontaneous-emission lifetime (0.67 ns). (a) Very low pump energy. (b) At high pump energy 2 µJ a pulse of 20ps duration is emitted; the height of this pulse is 2500 times stronger than that shown in (a).

Fig. 4
Fig. 4

Dynamics of the double-pass configuration: (a) low pump energy 0.4 µJ, (b) higher pump energy 0.8 µJ. In both cases the first and second peaks represent light that makes a single and a double pass, respectively, through the gain medium.

Fig. 5
Fig. 5

Dynamics of the laser (a) just below and (b) far above threshold. The output of the laser consists of two interleaved pulse trains representing light circulating in opposite directions through the cavity. The cavity round-trip time τcav200 ps is indicated.

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