Abstract

We report a new approach that uses the single beam Z-scan technique, to discriminate between excited state absorption (ESA) and two and three photon nonlinear absorption. By measuring the apparent delay or advance of the pulse in reaching the detector, the nonlinear absorption can be unambiguously identified as either instantaneous or transient. The simple method does not require a large range of input fluences or sophisticated pulse-probe experimental apparatus. The technique is easily extended to any absorption process dependent on pulse width and to nonlinear refraction measurements. We demonstrate in particular, that the large nonlinear absorption in ZnO nanocones when exposed to nanosecond 532 nm pulses, is due mostly to ESA, not pure two-photon absorption.

© 2014 Optical Society of America

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References

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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]

2013 (1)

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

2012 (1)

J. Chang, E. R. Waclawik, “Facet-controlled self-assembly of ZnO nanocrystals by non-hydrolytic aminolysis and their photodegradation activities,” CrystEngComm 14(11), 4041 (2012).
[CrossRef]

2011 (1)

2010 (1)

2009 (2)

C. Zhang, F. Zhang, T. Xia, N. Kumar, J. I. Hahm, J. Liu, Z. L. Wang, J. Xu, “Low-threshold two-photon pumped ZnO nanowire lasers,” Opt. Express 17(10), 7893–7900 (2009).
[CrossRef] [PubMed]

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

2008 (2)

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

B. Gu, Y. Sun, W. Ji, “Two-photon-induced excited-state nonlinearities,” Opt. Express 16(22), 17745–17751 (2008).
[CrossRef] [PubMed]

1997 (2)

T. Xia, D. J. Hagan, A. Dogariu, A. A. Said, E. W. Van Stryland, “Optimization of optical limiting devices based on excited-state absorption,” Appl. Opt. 36(18), 4110–4122 (1997).
[CrossRef] [PubMed]

X. Zhang, H. Fang, S. Tang, W. Ji, “Determination of two-photon-generated free-carrier lifetime in semiconductors by a single-beam Z-scan technique,” Appl. Phys. B Lasers Opt. 65(4-5), 549–554 (1997).
[CrossRef]

1996 (1)

1992 (1)

1990 (1)

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

Caplan, D. O.

Chang, J.

J. Chang, E. R. Waclawik, “Facet-controlled self-assembly of ZnO nanocrystals by non-hydrolytic aminolysis and their photodegradation activities,” CrystEngComm 14(11), 4041 (2012).
[CrossRef]

Cui, Y. P.

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

Deepthy, A.

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

Dogariu, A.

Fang, H.

X. Zhang, H. Fang, S. Tang, W. Ji, “Determination of two-photon-generated free-carrier lifetime in semiconductors by a single-beam Z-scan technique,” Appl. Phys. B Lasers Opt. 65(4-5), 549–554 (1997).
[CrossRef]

Fujita, Y.

Gopinath, P.

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

Gu, B.

Hagan, D. J.

T. Xia, D. J. Hagan, A. Dogariu, A. A. Said, E. W. Van Stryland, “Optimization of optical limiting devices based on excited-state absorption,” Appl. Opt. 36(18), 4110–4122 (1997).
[CrossRef] [PubMed]

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

Hahm, J. I.

Haripadmam, P. C.

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

Irimpan, L.

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

Ji, W.

John, H.

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

Kanter, G. S.

Kavitha, M. K.

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

Krishnan, B.

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

Kumar, N.

Kumar, O.

Kumar, P.

Lin, J.

Liu, J.

Lou, K.

Lv, C. G.

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

Mansour, K.

Nampoori, V. P. N.

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

Neogi, A.

Radhakrishnan, P.

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

Said, A.

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

Said, A. A.

Senthilkumar, K.

Sheik-Bahae, M.

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

Soileau, M. J.

Sun, Y.

Tang, S.

X. Zhang, H. Fang, S. Tang, W. Ji, “Determination of two-photon-generated free-carrier lifetime in semiconductors by a single-beam Z-scan technique,” Appl. Phys. B Lasers Opt. 65(4-5), 549–554 (1997).
[CrossRef]

Urban, B. E.

Van Stryland, E. W.

Waclawik, E. R.

J. Chang, E. R. Waclawik, “Facet-controlled self-assembly of ZnO nanocrystals by non-hydrolytic aminolysis and their photodegradation activities,” CrystEngComm 14(11), 4041 (2012).
[CrossRef]

Wang, H. T.

Wang, Z. L.

Wei, T. H.

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

Xia, T.

Xu, C. X.

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

Xu, J.

Zhang, C.

Zhang, F.

Zhang, X.

X. Zhang, H. Fang, S. Tang, W. Ji, “Determination of two-photon-generated free-carrier lifetime in semiconductors by a single-beam Z-scan technique,” Appl. Phys. B Lasers Opt. 65(4-5), 549–554 (1997).
[CrossRef]

Zhu, G. P.

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

Zhu, J.

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. B Lasers Opt. (1)

X. Zhang, H. Fang, S. Tang, W. Ji, “Determination of two-photon-generated free-carrier lifetime in semiconductors by a single-beam Z-scan technique,” Appl. Phys. B Lasers Opt. 65(4-5), 549–554 (1997).
[CrossRef]

Appl. Phys. Lett. (1)

G. P. Zhu, C. X. Xu, J. Zhu, C. G. Lv, Y. P. Cui, “Two-photon excited whispering-gallery mode ultraviolet laser from an individual ZnO microneedle,” Appl. Phys. Lett. 94(5), 051106 (2009).
[CrossRef]

CrystEngComm (1)

J. Chang, E. R. Waclawik, “Facet-controlled self-assembly of ZnO nanocrystals by non-hydrolytic aminolysis and their photodegradation activities,” CrystEngComm 14(11), 4041 (2012).
[CrossRef]

IEEE J. Quantum Electron. (1)

M. Sheik-Bahae, A. Said, T. H. Wei, D. J. Hagan, E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[CrossRef]

J. Appl. Phys. (1)

L. Irimpan, V. P. N. Nampoori, P. Radhakrishnan, B. Krishnan, A. Deepthy, “Size-dependent enhancement of nonlinear optical properties in nanocolloids of ZnO,” J. Appl. Phys. 103(3), 033105 (2008).
[CrossRef]

J. Opt. Soc. Am. B (1)

Mater. Res. Bull. (1)

M. K. Kavitha, P. C. Haripadmam, P. Gopinath, B. Krishnan, H. John, “Effect of morphology and solvent on two-photon absorption of nano zinc oxide,” Mater. Res. Bull. 48, 1967–1971 (2013).
[CrossRef]

Opt. Express (2)

Opt. Lett. (2)

Opt. Mater. Express (1)

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Figures (7)

Fig. 1
Fig. 1

Pulse deformation under 2PA, 3PA, and 2PA induced ESA keeping the nonlinear absorption at a constant 20%. (a) and (b) show the input and output pulses for a Gaussian and skew-normal temporal distributions respectively. (c) and (d) give the change in pulse delay as a function of transmission for Gaussian and skew-normal temporal distributions respectively. σ is the standard deviation of the input pulse.

Fig. 2
Fig. 2

Experimental set-up for Z-scan measurements.

Fig. 3
Fig. 3

Optical extinction spectrum (at a concentration of 0.1 mg/ml) and SEM image of ZnO nanocones.

Fig. 4
Fig. 4

Z-scan traces and single parameter least square fits of a 0.2 mg/ml ZnO nanocones sample at (a) 1.32 and (b) 0.87 GW/cm2.

Fig. 5
Fig. 5

Fitted values of (a) α 2 , and (b) α E S A , normalized by the ZnO concentration. The error bars give the 95% confidence intervals.

Fig. 6
Fig. 6

Experimental pulse delay measurements for the Z-scans of 0.2 mg/ml ZnO nanocones sample at (a) 1.32 and (b) 0.87 GW/cm2. The lines are the results of the single parameter least square fits from the Z-scan traces in Fig. 3.

Fig. 7
Fig. 7

Collation of all 6 Z-scan experiments is given. The theoretical curves for pure 2PA, 3PA and ESA are shown as solid lines.

Equations (4)

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

I z = ( α 0 + α 2 I + α 3 I 2 ) I
α 3 = α E S A G ( t ) = ϕ σ e α 2 2 h ν G ( t )
G ( t ) = 1 I t 2 ( t ) t I t 2 ( t ) d t
δ t = t I e ( t ) d t I e ( t ) d t

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