Abstract

We present what we believe to be the first experimental determination of the third-order optical susceptibility χ(3) of bulk cuprous oxide (Cu2O) crystals. The measured nonlinear refractive index, obtained with the Z-scan technique at 1064nm, is n2=1.32×1010esu, while the two-photon absorption coefficient is β=5.0cmGW of Cu2O. We also observe strong third-harmonic generation (THG) from Cu2O in our detection range owing to its unique crystal and electronic structure. Considering that the first nonvanishing nonlinear term is χ(3), this classical semiconductor could be utilized as a promising active THG medium.

© 2009 Optical Society of America

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  1. D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
    [CrossRef]
  2. J. I. Jang and J. P. Wolfe, Phys. Rev. B 74, 045211 (2006).
    [CrossRef]
  3. J. I. Jang and J. B. Ketterson, Solid State Commun. 146, 128 (2008).
    [CrossRef]
  4. See, for example, K. E. O'Hara, Ph.D. thesis (University of Illinois, 1999) and references therein.
  5. J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
    [CrossRef]
  6. K. Yoshioka and M. Kuwata-Gonokami, Phys. Rev. B 73, 081202(R) (2006).
    [CrossRef]
  7. D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
    [CrossRef] [PubMed]
  8. W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
    [CrossRef]
  9. M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
    [CrossRef]
  10. M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
    [CrossRef]
  11. S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
    [CrossRef]
  12. A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
    [CrossRef]
  13. K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
    [CrossRef]
  14. T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
    [CrossRef] [PubMed]

2009 (1)

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

2008 (3)

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

J. I. Jang and J. B. Ketterson, Solid State Commun. 146, 128 (2008).
[CrossRef]

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

2006 (2)

K. Yoshioka and M. Kuwata-Gonokami, Phys. Rev. B 73, 081202(R) (2006).
[CrossRef]

J. I. Jang and J. P. Wolfe, Phys. Rev. B 74, 045211 (2006).
[CrossRef]

2002 (1)

A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
[CrossRef]

1999 (2)

K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
[CrossRef]

See, for example, K. E. O'Hara, Ph.D. thesis (University of Illinois, 1999) and references therein.

1996 (1)

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

1991 (1)

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

1990 (1)

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

1985 (1)

D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
[CrossRef] [PubMed]

1980 (1)

D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
[CrossRef]

Benoît à la Guillaume, C.

D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
[CrossRef]

Bing-suo, Z.

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

Fröhlich, D.

D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
[CrossRef] [PubMed]

Gullingsrud, J. R.

K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
[CrossRef]

Hagan, D. J.

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Hulin, D.

D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
[CrossRef]

Hutchings, D. C.

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

Ideguchi, T.

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

Jang, J. I.

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

J. I. Jang and J. B. Ketterson, Solid State Commun. 146, 128 (2008).
[CrossRef]

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

J. I. Jang and J. P. Wolfe, Phys. Rev. B 74, 045211 (2006).
[CrossRef]

Jiang, Z.

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

Jin-hai, S.

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

Jöger, M.

A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
[CrossRef]

Jolk, A.

A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
[CrossRef]

Ketterson, J. B.

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

J. I. Jang and J. B. Ketterson, Solid State Commun. 146, 128 (2008).
[CrossRef]

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

Klingshirn, C.

A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
[CrossRef]

Kuwata-Gonokami, M.

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

K. Yoshioka and M. Kuwata-Gonokami, Phys. Rev. B 73, 081202(R) (2006).
[CrossRef]

Mani, S.

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

Mysyrowicz, A.

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
[CrossRef]

Nöthe, A.

D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
[CrossRef] [PubMed]

O'Hara, K. E.

See, for example, K. E. O'Hara, Ph.D. thesis (University of Illinois, 1999) and references therein.

K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
[CrossRef]

Park, H. Y.

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

Pei-xians, Y.

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

Reimann, K.

D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
[CrossRef] [PubMed]

Said, A. A.

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Sheik-Bahae, M.

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Sun, Y.

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

Van Stryland, E. W.

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Wei, T.

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Wolfe, J. P.

J. I. Jang and J. P. Wolfe, Phys. Rev. B 74, 045211 (2006).
[CrossRef]

K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
[CrossRef]

Yoshioka, K.

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

K. Yoshioka and M. Kuwata-Gonokami, Phys. Rev. B 73, 081202(R) (2006).
[CrossRef]

You-gui, W.

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

Appl. Phys. Lett. (1)

J. I. Jang, Y. Sun, S. Mani, and J. B. Ketterson, Appl. Phys. Lett. 93, 121111 (2008).
[CrossRef]

Chin. Phys. Lett. (1)

W. You-gui, S. Jin-hai, Z. Jiang, Z. Bing-suo, and Y. Pei-xians, Chin. Phys. Lett. 13, 182 (1996).
[CrossRef]

IEEE J. Quantum Electron. (2)

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, IEEE J. Quantum Electron. 27, 1296 (1991).
[CrossRef]

J. Cryst. Growth (1)

S. Mani, J. I. Jang, J. B. Ketterson, and H. Y. Park, J. Cryst. Growth 311, 3549 (2009).
[CrossRef]

Phys. Rev. B (4)

A. Jolk, M. Jöger, and C. Klingshirn, Phys. Rev. B 65, 245209 (2002).
[CrossRef]

K. E. O'Hara, J. R. Gullingsrud, and J. P. Wolfe, Phys. Rev. B 60, 10872 (1999).
[CrossRef]

K. Yoshioka and M. Kuwata-Gonokami, Phys. Rev. B 73, 081202(R) (2006).
[CrossRef]

J. I. Jang and J. P. Wolfe, Phys. Rev. B 74, 045211 (2006).
[CrossRef]

Phys. Rev. Lett. (3)

D. Fröhlich, A. Nöthe, and K. Reimann, Phys. Rev. Lett. 55, 1335 (1985).
[CrossRef] [PubMed]

T. Ideguchi, K. Yoshioka, A. Mysyrowicz, and M. Kuwata-Gonokami, Phys. Rev. Lett. 100, 233001 (2008).
[CrossRef] [PubMed]

D. Hulin, A. Mysyrowicz, and C. Benoît à la Guillaume, Phys. Rev. Lett. 45, 1970 (1980).
[CrossRef]

Solid State Commun. (1)

J. I. Jang and J. B. Ketterson, Solid State Commun. 146, 128 (2008).
[CrossRef]

Other (1)

See, for example, K. E. O'Hara, Ph.D. thesis (University of Illinois, 1999) and references therein.

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Figures (4)

Fig. 1
Fig. 1

Normalized closed-aperture Z-scan data obtained from a Cu 2 O sample with 20% aperture transmittance. Inset, plot of Δ n versus I for a synthetic Cu 2 O sample. A similar linear relationship was observed from the natural-growth sample.

Fig. 2
Fig. 2

Open-aperture Z-scan data ( S = 1 ) .

Fig. 3
Fig. 3

(a) Wavelength-dependent third-harmonic generation (THG) from Cu 2 O (upper curves) and GaAs (lower curves). (b) Corresponding second-harmonic generation (SHG) signals from GaAs. We confirmed that there is no SHG response from Cu 2 O .

Fig. 4
Fig. 4

Low-temperature THG-wavelength scan around the two-photon resonance.

Equations (3)

Equations on this page are rendered with MathJax. Learn more.

Δ T 0.406 ( 1 S ) 0.25 2 π λ L eff Δ n ,
n 2 = K E p n 0 E g 4 G 2 ( ω E g ) ,
β ( ω ) = K E p n 0 2 E g 3 F 2 ( ω E g ) ,

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