Abstract

Bound-electronic and free-carrier optical nonlinearities and relaxation of two-photon-excited free carriers in ZnO have been investigated by use of a single-beam Z-scan technique at 532 nm. Under pulsed radiation of 25-ps duration, the two-photon absorption coefficient, the bound-electron nonlinear refractive index, and the change in the refractive index due to the two-photon generation of an electron–hole pair are determined to be 4.2±0.9 cm/GW, -(0.9±0.3)×10-14 cm2/W, and -(1.1±0.3)×10-21 cm3, respectively. With these values in the Z scans conducted with 7-ns laser pulses, the carrier recombination time and the free-carrier absorption cross section are extracted as 2.8±0.6 ns and (6.5±0.9)×10-18 cm2, respectively.

© 1997 Optical Society of America

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References

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  1. E. C. Fox and H. M. van Driel, “Femtosecond probing of photoinduced refractive index changes in semiconductors,” in Ultrashort Processes in Condensed Matter, W. E. Born ed. (Plenum, New York, 1993), pp. 1–51.
  2. M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
    [CrossRef]
  3. A. A. Said, M. Sheik-Bahae, D. J. Hagan, T. H. Wei, J. Wang, J. Young, and E. W. Van Stryland, “Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe,” J. Opt. Soc. Am. B 9, 405–414 (1992).
    [CrossRef]
  4. K. Lee, W. Cho, J. Park, J. Kim, S. Park, and U. Kim, “Measurement of free-carrier nonlinearities in ZnSe based on the Z-scan technique with a nanosecond laser,” Opt. Lett. 19, 1116–1118 (1994).
    [CrossRef] [PubMed]
  5. T. D. Krauss and F. W. Wise, “Femtosecond measurement of nonlinear absorption and refraction in CdS, ZnSe, and ZnS,” Appl. Phys. Lett. 65, 1739–1741 (1994).
    [CrossRef]
  6. J. Wang, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Time-resolved Z-scan measurements of optical nonlinearities,” J. Opt. Soc. Am. B 11, 1009–1017 (1994).
    [CrossRef]
  7. K. Y. Tseng, K. S. Wong, and G. K. L. Wong, “Femtosecond time-resolved Z-scan investigations of optical nonlinearities in ZnSe,” Opt. Lett. 21, 180–182 (1996).
    [CrossRef] [PubMed]
  8. D. R. Dean and R. J. Collins, “Transient phase gratings in ZnO induced by two-photon absorption,” J. Appl. Phys. 44, 5455–5457 (1973).
    [CrossRef]
  9. H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
    [CrossRef]
  10. J. N. Ravn, “Laser-induced grating in ZnO,” IEEE J. Quantum Electron. 28, 315–322 (1992).
    [CrossRef]
  11. R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
    [CrossRef]
  12. J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
    [CrossRef]
  13. K. H. Hellwege, Landolt-Bornstein Numerical Data and Functional Relationships in Science and Technology, Vol. 17 of Semiconductors (Springer-Verlag, New York, 1982), Subvol. (b).
  14. M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
    [CrossRef]

1996 (1)

1994 (3)

1993 (1)

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

1992 (2)

1991 (1)

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

1990 (1)

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

1989 (1)

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
[CrossRef]

1986 (1)

H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
[CrossRef]

1973 (1)

D. R. Dean and R. J. Collins, “Transient phase gratings in ZnO induced by two-photon absorption,” J. Appl. Phys. 44, 5455–5457 (1973).
[CrossRef]

Adair, R.

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
[CrossRef]

Bolger, J. A.

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

Chase, L. L.

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
[CrossRef]

Cho, W.

Collins, R. J.

D. R. Dean and R. J. Collins, “Transient phase gratings in ZnO induced by two-photon absorption,” J. Appl. Phys. 44, 5455–5457 (1973).
[CrossRef]

Dean, D. R.

D. R. Dean and R. J. Collins, “Transient phase gratings in ZnO induced by two-photon absorption,” J. Appl. Phys. 44, 5455–5457 (1973).
[CrossRef]

DeSalvo, R.

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

Hagan, D. J.

J. Wang, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Time-resolved Z-scan measurements of optical nonlinearities,” J. Opt. Soc. Am. B 11, 1009–1017 (1994).
[CrossRef]

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

A. A. Said, M. Sheik-Bahae, D. J. Hagan, T. H. Wei, J. Wang, J. Young, and E. W. Van Stryland, “Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe,” J. Opt. Soc. Am. B 9, 405–414 (1992).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

Hutchings, D. C.

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

Kalt, H.

H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
[CrossRef]

Kar, A. K.

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

Kim, J.

Kim, U.

Klingshirn, C.

H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
[CrossRef]

Krauss, T. D.

T. D. Krauss and F. W. Wise, “Femtosecond measurement of nonlinear absorption and refraction in CdS, ZnSe, and ZnS,” Appl. Phys. Lett. 65, 1739–1741 (1994).
[CrossRef]

Lee, K.

Park, J.

Park, S.

Payne, S. A.

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
[CrossRef]

Ravn, J. N.

J. N. Ravn, “Laser-induced grating in ZnO,” IEEE J. Quantum Electron. 28, 315–322 (1992).
[CrossRef]

Renner, R.

H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
[CrossRef]

Said, A. A.

Sheik-Bahae, M.

J. Wang, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Time-resolved Z-scan measurements of optical nonlinearities,” J. Opt. Soc. Am. B 11, 1009–1017 (1994).
[CrossRef]

A. A. Said, M. Sheik-Bahae, D. J. Hagan, T. H. Wei, J. Wang, J. Young, and E. W. Van Stryland, “Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe,” J. Opt. Soc. Am. B 9, 405–414 (1992).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

Tseng, K. Y.

Van Stryland, E. W.

J. Wang, M. Sheik-Bahae, A. A. Said, D. J. Hagan, and E. W. Van Stryland, “Time-resolved Z-scan measurements of optical nonlinearities,” J. Opt. Soc. Am. B 11, 1009–1017 (1994).
[CrossRef]

A. A. Said, M. Sheik-Bahae, D. J. Hagan, T. H. Wei, J. Wang, J. Young, and E. W. Van Stryland, “Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe,” J. Opt. Soc. Am. B 9, 405–414 (1992).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

Wang, J.

Wei, T. H.

A. A. Said, M. Sheik-Bahae, D. J. Hagan, T. H. Wei, J. Wang, J. Young, and E. W. Van Stryland, “Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe,” J. Opt. Soc. Am. B 9, 405–414 (1992).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

Wherrett, B. S.

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

Wise, F. W.

T. D. Krauss and F. W. Wise, “Femtosecond measurement of nonlinear absorption and refraction in CdS, ZnSe, and ZnS,” Appl. Phys. Lett. 65, 1739–1741 (1994).
[CrossRef]

Wong, G. K. L.

Wong, K. S.

Young, J.

Appl. Phys. Lett. (1)

T. D. Krauss and F. W. Wise, “Femtosecond measurement of nonlinear absorption and refraction in CdS, ZnSe, and ZnS,” Appl. Phys. Lett. 65, 1739–1741 (1994).
[CrossRef]

IEEE J. Quantum Electron. (4)

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[CrossRef]

H. Kalt, R. Renner, and C. Klingshirn, “Resonant self-diffraction from dynamic, laser-induced gratings in II–VI compounds,” IEEE J. Quantum Electron. QE-22, 1312–1319 (1986).
[CrossRef]

J. N. Ravn, “Laser-induced grating in ZnO,” IEEE J. Quantum Electron. 28, 315–322 (1992).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of bound electronic nonlinear refraction in solids,” IEEE J. Quantum Electron. 27, 1296–1309 (1991).
[CrossRef]

J. Appl. Phys. (1)

D. R. Dean and R. J. Collins, “Transient phase gratings in ZnO induced by two-photon absorption,” J. Appl. Phys. 44, 5455–5457 (1973).
[CrossRef]

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

Opt. Commun. (1)

J. A. Bolger, A. K. Kar, B. S. Wherrett, R. DeSalvo, D. C. Hutchings, and D. J. Hagan, “Nondegenerate two-photon absorption spectra of ZnSe, ZnS and ZnO,” Opt. Commun. 97, 203–209 (1993).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. B (1)

R. Adair, L. L. Chase, and S. A. Payne, “Nonlinear refrac- tive index of optical crystals,” Phys. Rev. B 39, 3337–3350 (1989).
[CrossRef]

Other (2)

E. C. Fox and H. M. van Driel, “Femtosecond probing of photoinduced refractive index changes in semiconductors,” in Ultrashort Processes in Condensed Matter, W. E. Born ed. (Plenum, New York, 1993), pp. 1–51.

K. H. Hellwege, Landolt-Bornstein Numerical Data and Functional Relationships in Science and Technology, Vol. 17 of Semiconductors (Springer-Verlag, New York, 1982), Subvol. (b).

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Figures (4)

Fig. 1
Fig. 1

Z scans conducted on a 1-mm-thick ZnO crystal. The open circles are the Z scans obtained (a) without and (b) with an aperture (S=0.5). The solid curves are calculated with the model described in the text. The data in (a) are vertically shifted by 0.3 for presentation.

Fig. 2
Fig. 2

Measured TPA coefficients (open circles) versus peak irradiances and Δn/Ip (filled circles) directly derived from ΔTpv plotted as a function of Ip for the ZnO crystal. The horizontal dashed line is a guide for the eye. The intercept of the linear best fit to the data gives γ=-0.9×10-14 cm2/W, and the slope yields σn=-1.1×10-21 cm3.

Fig. 3
Fig. 3

Z scans performed on the ZnO sample. The open circles are the Z scans (a) without and (b) with an aperture (S=0.2). The filled circles (c) are obtained from dividing the data in (a) by the results in (b). The curves are calculated by the model described in the text. The data in (a) and (b) are vertically shifted by 0.4 and 0.2, respectively, for presentation.

Fig. 4
Fig. 4

Calculated change in the refractive index per unit free-carrier density as a function of the free-carrier density. The values listed in the figure are used in the calculation and are quoted from Ref. 13.

Tables (1)

Tables Icon

Table 1 Comparison of Nonlinear Parameters for ZnO and ZnSe

Equations (4)

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dΔϕ/dz=k(γI+σnΔN),
dI/dz=-α0I,
dΔN/dt=βI2/2ω-ΔN/τ,
dI/dz=-(α0+βI+σαΔN)I.

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