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Three-photon absorption in ZnO and ZnS crystals

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Abstract

We report a systematic investigation of both three-photon absorption (3PA) spectra and wavelength dispersions of Kerr-type nonlinear refraction in wide-gap semiconductors. The Z-scan measurements are recorded for both ZnO and ZnS with femtosecond laser pulses. While the wavelength dispersions of the Kerr nonlinearity are in agreement with a two-band model, the wavelength dependences of the 3PA are found to be given by (3E photon/Eg -1)5/2(3E photon/Eg )-9. We also evaluate higher-order nonlinear optical effects including the fifth-order instantaneous nonlinear refraction associated with virtual three-photon transitions, and effectively seventh-order nonlinear processes induced by three-photon-excited free charge carriers. These higher-order nonlinear effects are insignificant with laser excitation irradiances up to 40 GW/cm2. Both pump-probe measurements and three-photon figures of merits demonstrate that ZnO and ZnS should be a promising candidate for optical switching applications at telecommunication wavelengths.

©2005 Optical Society of America

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Figures (7)

Fig. 1.
Fig. 1. (a) OA Z-scans measured with different excitation irradiances at a wavelength of 780 nm and a pulse repetition rate of 90 MHz. The solid and dashed lines are the fitting curves by employing the Z-scan theory, described in the text, on 3PA and 2PA respectively. (b) Plots of Ln(1-T OA) vs. Ln(I 0) at different wavelengths, the solid lines are the examples of the linear fit at 740 nm with a slope of s = 0.86 and at 840 nm with a slope of s = 1.96.
Fig. 2.
Fig. 2. 3PA coefficients plotted as a function of E photon/Eg , where E photon is the photon energy and Eg is the band-gap energy. The solid stars and squares are the experimental data, while the solid and dashed lines are calculated from the theory of Brandi and de Araujo [19] and the theory of Wherrett [25], respectively. For comparison, the experimental result (the empty square) of Catalano et al. is also displayed [17].
Fig. 3.
Fig. 3. (a) OA Z-scans and (b) CA Z-scans divided by OA Z-scans measured with 1-kHz repetition rate laser pulses at various excitation irradiances. The inset in (a) and (b) shows the irradiance dependence of the 3PA coefficient and the irradiance dependence of the n 2 value, respectively.
Fig. 4.
Fig. 4. (a) OA Z-scan, CA Z-scan and CA Z-scan divided by OA Z-scan; and (b) Kerr-type nonlinear refraction plotted as a function of E photon/Eg . The solid scatters are the experimental data, while the solid lines are calculated from the theory of Sheik-Bahae et al. [26]. For comparison, the experimental results of Adair et al. (the empty triangles) [5], Zhang et al. (the empty square) [6], and Krauss et al. (the empty circles) [7], are also displayed.
Fig. 5.
Fig. 5. Calculated nonlinear refraction n 4 plotted against E photon/Eg , for both ZnO (the dashed line) and ZnS (the solid line).
Fig. 6.
Fig. 6. Calculated nonlinear refraction changes (n 2 I, n 4 I 2, σ r N e-h) vs. the irradiance for (a) ZnO and (b) ZnS; and calculated changes in nonlinear absorption (α 3 I 2, σ a N e-h) vs. the irradiance for (c) ZnO and (d) ZnS. Herein, wavelength is 780 nm, n 2 is 1.0 × 10-5 cm2/GW (0.69 × 10-5 cm2/GW), n 4 is -1.4 × 10-26 cm4/W2 (3.1 × 10-27 cm4/W2), α 3 is 0.016 cm3/GW2 (0.0021 cm3/GW2) for ZnO (ZnS) crystal, and α r = -1.1×10-21 cm3 and σ a = 6.5×10-18 cm2 are assumed for both ZnO and ZnS crystals [6].
Fig. 7.
Fig. 7. Normalized OKE signal (the solid squares for ZnO) and pump-probe signals (the solid stars for ZnO and the solid circles for ZnS) measured at a wavelength of 780 nm as a function of the delay time. The experiment data were measured under the same excitation irradiance (~ 9.0 GW/cm2) with 1-kHz pulse repetition rate. The dashed line and solid lines are the 2PA and 3PA intensity autocorrelation functions of the laser pulses, respectively.

Tables (1)

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Table 1. Measured 3PA or 2PA coefficient, Kerr-type refractive nonlinearity, and calculated nonlinear FOM for ZnO and ZnS. The relative errors are estimated as ±20%

Equations (12)

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d Δ ϕ dz = k m = 2 n 2 m 2 I m 1 + r N e h
dI dz = ( α 0 + m = 2 α m I m 1 + σ a N e h ) I
T OA ( z ) = 1 π 1 2 q 0 ln [ 1 + q 0 exp ( x 2 ) ] dx
T OA ( z ) = 1 π 1 2 p 0 ln { [ 1 + p 0 2 exp ( 2 x 2 ) ] 1 2 + p 0 exp ( x 2 ) } dx
T OA = m = 0 ( 1 ) m q 0 m ( m + 1 ) 3 2
T OA = m = 1 ( 1 ) m 1 p 0 2 m 2 ( 2 m 1 ) ! ( 2 m 1 ) 1 2
T OA = 1 α 2 I 0 L eff 2 3 2
T OA = 1 α 3 I 0 2 L eff 3 3 2
α 3 = 3 10 2 1 2 8 π 2 ( e 2 ħc ) 3 ħ 2 P 3 n 0 3 E g 7 ( 3 E photon E g 1 ) 1 2 ( 3 E photon E g ) 9
α 3 = 2 9 2 3 10 π 2 5 ( e 2 ħc ) 3 ħ 2 S 3 ( 3 E photon E g 1 ) 5 2 ( 3 E photon E g ) 9
n 4 ω 1 ω 2 ω 3 = c π 0 α 3 ( Ω ; ω 2 , ω 3 ) Ω 2 ω 1 2 d Ω
dN e h dt = α 3 I 3 3 ħω N e h τ
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