Study of the third order nonlinear optical properties of Zn<Subscript>1−x</Subscript>Mg<Subscript>x</Subscript>Se and Cd<Subscript>1−x</Subscript>Mg<Subscript>x</Subscript>Se crystals

Third order nonlinear optical susceptibilities χ^<3> of ternary Zn_1−xMg_xSe and Cd_1−xMg_xSe crystals have been measured using standard degenerate four-wave mixing (DFWM) method at 532 nm. The nonlinear transmission technique has been applied to check if our crystals exhibit two-photon absorption. The studied Zn_1−xMg_xSe and Cd_1−xMg_xSe solid solutions were grown from the melt by the modified high-pressure Bridgman method. For both crystals the energy gap increases with increasing Mg content. In the case of Zn_1−xMg_xSe, it was found that the value of third order nonlinear optical susceptibility χ^<3> decreases with increasing Mg content. An explanation of this behaviour results from the dependence of optical nonlinearities on the energy band gap E_g of the studied crystals. In the case of Cd_1txMg_xSe with low content of Mg, no response was observed for the studied wavelength since the energy gap in such crystals is smaller than the photon energy of the used laser radiation. It was also found that the value of third order nonlinear optical susceptibility χ^<3> for Cd_0.70Mg_0.30Se is higher than for Zn_0.67Mg_0.33Se. This behaviour can be understood if one take into consideration that the free carrier concentration in Cd_1−xMg_xSe samples is about four orders of magnitude higher than that in Zn_1txMg_xSe ones with comparable Mg content respectively. It is commonly known that when the electric conductivity increases, the values of nonlinear optical properties increase. From the performed measurements one can conclude that the incorporation of Mg as constituent into ZnSe and CdSe crystals leads to a change of the third order nonlinear optical susceptibilities.     

GaS0.4Se0.6: Relevant properties and potential for 1064 nm pumped mid-IR OPOs and OPGs operating above 5 μm

We present measurements of the transparency, refractive index dispersion, nonlinear coefficient, damage threshold, and two-photon absorption of mixed GaS _x Se_{1 − x} crystals and show that GaS_0.4Se_0.6 is a promising nonlinear material for down conversion of pulsed 1064 nm radiation to the mid-IR above 5 μm without significant two-photon absorption.     

Properties of optical phonons in Zn1−x−yMgyBexSe quaternary mixed crystal

Long wavelength optical lattice vibration and dielectric constants of the quaternary mixed crystal Zn_1−x−yMg_yBe_xSe are investigated based on the pseudo-unit-cell mode and Born-Huang procedure. It is found that this material shows a three-mode behavior and the oscillator strength of each mode is mainly controlled by only one component. The theoretical results also show that the linear interpretation method for dielectric constants is reliable. The vibrational frequencies and the oscillator strengths of the ternary mixed crystals Be_xZn_1−xSe, Be_xMg_1−xSe and Mg_xZn_1−xSe are also calculated as special cases of the quaternary mixed crystal for comparing with experiments. The calculation shows agreement with the experimental results.     

Azimuthal dependence of the two-photon absorption coefficient for CdP2 crystals with tetragonal syngony

We studied the two-photon absorption coefficient (β) for cadmium diphosphide (CdP₂) single crystals in the tetragonal modification vs. the polarization azimuth (φ) of the incident light for intensities close to the optical breakdown (or optical damage) threshold for the crystal (11 MW/cm²). We have established that the value of β_max = 0.16 cm/MW is reached for φ = 0, i.e., for the ordinary wave. At the lasing frequency of a ruby laser, β_⊥/β_|| = 2.13, which suggests anisotropy of the two-photon absorption in the studied crystals. These dependences are needed for design and fabrication of quantum electronics and nonlinear optics elements whose operation is based on the use of the two-photon absorption effect for high radiation fluxes. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 76, No. 1, pp. 117–121, January–February, 2009.     

Large near resonance third order nonlinearity in GaN

We have studied third order nonlinearities, including two-photon absorption coefficient and nonlinear refractive index n ₂, of GaN in below bandgap ultraviolet (UV) wavelength regime by using UV femtosecond pulses. Two-photon absorption was investigated by demonstrating femtosecond UV pulsewidth autocorrelation in a GaN thin film while femtosecond Z-scan measurements revealed information for both n ₂ and . The distribution of n ₂ versus wavelength was found to be consistent with a model described by the quadratic Stark effect, which is the dominant factor contributed to the nonlinear refractive index near the bandgap. Large on the order of 10 cm/GW and large negative n ₂ with a magnitude on the order of several 10^–12 cm²/W were obtained. The at near mid-gap infrared (IR) wavelength was also found to be on the order of several cm/GW by using two-photon-type autocorrelations in a GaN thin film. Taking advantage of the large two-photon absorption at mid-gap wavelengths, we have demonstrated excellent image quality on two-photon confocal microscopy, including two-photon-scanning-photoluminescence imaging and two-photon optical-beam-induced current microscopy, on a GaN Hall measurement sample and an InGaN green light emitting diode.     

Photoacoustic method of determination of quantum efficiency of luminescence in Mn<Superscript>2+</Superscript> ions in Zn<Subscript>1−x−y</Subscript>Be<Subscript>x</Subscript>Mn<Subscript>y</Subscript>Se crystals

This paper presents step by step the procedure of determination of the quantum efficiency of luminescence of Mn²⁺ ions in the Zn_1−x−yBe_xMn_ySe crystals. The method is based on the photoacoustic spectroscopy approach. In the paper, the experimental spectra of absorbance, transmission, absorption and photoacoustic spectra of the samples are presented and analyzed from the point of view of the possibility of determination of the quantum efficiency of Mn²⁺ ion luminescence at room temperature. It was determined experimentally that in the investigated crystals the quantum efficiency of luminescence in the Mn²⁺ ions is about 35%, 40%, 32% for the absorption peaks at 430 nm, 470 nm, and 510 nm, respectively, for Zn_0.75Be_0.2Mn_0.05Se crystal.     

Be-composition effect on structure, electronic and optical properties of BexZn1-xO alloys

This paper carries out first principles calculation of the structure,electronic and optical properties of Be x Zn 1 x O alloys based on the density-functional theory for the compositions x = 0.0,0.25,0.5,0.75,1.0.The lattice constants deviations of alloys obey Vegard’s law well.The Be x Zn 1 x O alloys have the direct band gap(Γ-Γ) character,and the bowing coefficients are less than the available theoretical values.Moreover,it investigates in detail the optical properties(dielectric functions,absorption spectrum and refractive index) of these ternary mixed crystals.The obtained results agree well with the available theoretical and experimental values.     

Two-photon absorption of high-power picosecond pulses in PbWO<Subscript>4</Subscript>, ZnWO<Subscript>4</Subscript>, PbMoO<Subscript>4</Subscript>, and CaMoO<Subscript>4</Subscript> crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm². The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO₄ and ZnWO₄ crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO₄ to β = 0.14 cm/GW for CaMoO₄, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.     

Nonlinear refraction of undoped and Fe-doped KTiOAsO4 crystals in the femtosecond regime

The third-order optical nonlinearities in undoped and Fe-doped KTA crystals have been measured using the Z-scan technique with femtosecond pulses at 780-nm wavelength. The nonlinear refractive index is determined to be 1.7×10⁻¹⁵ cm²/W and 0,9×10⁻¹⁵ cm²/W for undoped and Fe-doped KTA, respectively. No two-photon absorption occurs in these crystals. It is shown that doping with Fe₂O₃ could weaken refractive nonlinearity of KTA, suggesting that Fe:KTA will improve the performance of KTA in high-intensity femtosecond laser applications. In addition, the measured nonlinear index of refraction in KTA crystals is about five times lower than that predicted by the two-band theory. One of the reasons for the discrepancy is given as the applicable limit of the simple theory in which a two-parabolic band model has been assumed in the analysis. Received: 3 June 1999 / Published online: 20 October 1999     

A comparison between optically active CdZnSe/ZnSe and CdZnSe/ZnBeSe self-assembled quantum dots: effect of beryllium

The composition and size of optically active Cd_xZn_1−xSe/ZnSe quantum dots are estimated with a previously developed method. The results are then compared with those obtained for Cd_xZn_1−xSe/Zn_0.97Be_0.03Se QDs. We show that introducing Be into the barrier material enhances both Cd composition and quantum size effect of optically active quantum dots.     

Nonlinear optical absorption in Bi3TiNbO9 thin films using Z-scan?technique

Bi₃TiNbO₉ (BTN) thin films with layered perovskite structure were fabricated on fused silica by pulsed laser deposition. The XRD pattern revealed that the films are single-phase perovskite and highly (00l) textured. Their fundamental optical constants, such as band gap, linear refractive index, and linear absorption coefficient, were obtained by optical transmittance measurements. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The nonlinear optical absorption of the films was investigated by single beam Z-scan method at a wavelength of 800 nm with laser duration of 80 fs. We obtained the nonlinear absorption coefficient β=1.44×10⁻⁷ m/W. The results show that the BTN thin films are promising for applications in absorbing-type optical devices.     

z-Scan characterization of zwitterionic chromophores for optoelectronic switching

Single beam z-scan measurements have been made on films containing amorphous polycarbonate and the zwitterionic chromophore, PYR-3, that has a very high second order nonlinear optical (NLO) figure of merit. The third order NLO figure of merit is ≈1.6 at 1030 nm and is comparable to that found in organic compounds optimized for high n ₂ values. The two-photon absorption coefficient is 2.1×10⁻¹² m/W, which is very low and advantageous for NLO device applications. The third order NLO refractive index is −1.4×10⁻¹⁸ m²/W.     

Low-Temperature Anti-Stokes Luminescence in Zn1-xMgxSe Mixed Crystals

Investigations of photoluminescence and Raman scattering in the ternary Zn_1-xMg_xSe compounds at 4.2 K were performed both in the Stokes and anti-Stokes regions using cw laser excitation with various wavelengths within the transparency band of the crystals. The anti-Stokes luminescence was observed for the first time in the ternary Zn_1-xMg_xSe compounds. We have found variations in the shape and position of the Stokes and anti-Stokes luminescence bands with an increase in the band gap energy, which depends on magnesium content. We assume that the anti-Stokes emission is generated by two-step excitation via deep-level centers. It is shown that the low-temperature anti-Stokes photoluminescence can probe the spatial distribution profiles of impurities in the bulk of crystals.     

Nonlinear responses and optical limiting behavior of fast green FCF dye under a low power CW He-Ne laser irradiation

The nonlinear responses and optical limiting performance of a dye type acid, called fast green FCF, are investigated under irradiation of 35 mW continuous wave He-Ne Laser. The second order refractive index and nonlinear absorption coefficient are measured by use of z-Scan technique. The optical limiting behavior is investigated by transmission measurement through the sample. Linear absorption coefficient (α), nonlinear absorption coefficient (β) and second order refractive index (n₂) of fast green FCF are measured at different concentrations.     

Nonlinear optical characterization of LaEr(MoO<Subscript>4</Subscript>)<Subscript>3</Subscript> thin films using the <Emphasis Type="BoldItalic">Z</Emphasis> -scan technique

The nonlinear optical properties of thin films of LaEr(MoO₄)₃ were studied using a ∼30 ps Nd:YAG laser at 532 nm with a repetition rate of 250 Hz. Closed aperture Z-scan measurement revealed a negative nonlinearity in the LaEr(MoO₄)₃. The nonlinear refractive index γ=1.38×10^-10 cm²/W and nonlinear absorption coefficient β=16.8×10^-6 cm/W were calculated from the Z-scan data. The fluorescent upconversion spectra were recorded with 980 nm excitation. An optical switching mechanism based on nonlinear absorption is also presented experimentally. PACS 81.15.Fg; 77.84.Bw; 33.50.Dq; 42.70.Mp     

Intensity-induced nonlinear effects in UV window materials

Intensity-induced nonlinear effects in optical window materials have been investigated at 308 nm. The absolute two-photon absorption coefficients for fused silica, CaF₂, BaF₂, Al₂O₃ and ADP crystals have been measured by using a single 120 ps, transform-limited pulse from the second harmonic of a distributed feedback (DFB) dye laser. The nonlinear refractive index coefficient has been obtained from measurements of far-field intensity distributions.     

Elasticity, band structure, and piezoelectricity of BexZn1−xO alloys

Lattice constants, elasticity, band structure and piezoelectricity of hexagonal wide band gap Be_xZn_1−xO ternary alloys are calculated using first-principles methods. The alloys' lattice constants obey Vegard's law well. As Be concentration increases, the bulk modulus and Young's modulus of the alloys increase, whereas the piezoelectricity decreases. We predict that Be_xZn_1−xO/GaN/substrate (x=0.022) multilayer structure can be suitable for high-frequency surface acoustic wave device applications. Our calculated results are in good agreement with experimental data and other theoretical calculations.     

Picosecond Z-scan study of bound electronic Kerr effect in LiNbO3 crystal associated with two-photon absorption

3 crystal have been measured using Z-scan technique with picosecond pulses at 532 nm. The nonlinear absorption coefficient and nonlinear refractive index are determined to be 2.5×10^-10 cm/W and 5.3×10^-15 cm²/W, respectively. Both sign and magnitude of the measured refractive nonlinearity are considerably different from the reported Z-scan results in LiNbO₃ obtained with cw laser beam at 514 nm. The nonlinearities in LiNbO₃ induced by 532 nm picosecond pulses are believed to be mainly due to two-photon absorption and bound electronic Kerr effect associated with the two-photon absorption. Received: 4 July 1996     

Z-scan measurements of optical nonlinearity in acid blue 29 dye

The third order nonlinear optical properties of acid blue 29 solutions have been studied using Z-scan technique. Experiments are performed using a CW He–Ne laser at 632.8 nm wavelength and 3 mW power. The linear absorption coefficient α₀, nonlinear absorption coefficient β, nonlinear refractive index n₂, Re χ³, and Im χ³ are measured at three different concentrations. Our results show that higher concentration gives better nonlinear optical properties. Also, it was found that there is an increasing trend in the value of the nonlinear refractive index n₂ as the concentration increases.     

Fe2O3纳米微粒溶胶非线性光学特性的Z-扫描研究

利用Z扫描技术在透明区域研究了Fe₂O₃纳米微粒水溶胶和表面包覆有机溶胶的非线性光学特性，给出了非线性折射率γ、双光子吸收系数β、自由载流子折射系数σ_r和自由载流子吸收截面σ_ab等重要物理参数，讨论了自由载流子效应对Fe₂O₃纳米微粒非线性特性的影响 关键词：