Intra-excitonic relaxation dynamics in ZnO Appl. Phys. Lett. 99, 231910 (2011) Thermal diffusion of nitrogen into ZnO film deposited on InN/sapphire substrate by metal organic chemical vapor deposition J. Appl. Phys. 110, 113509 (2011) Manifestation of spin-spin interaction between oxygen vacancy and magnesium in ZnMgO nanorods by electron paramagnetic resonance studies Appl. Phys. Lett. 99, 194101 (2011) Selective pair luminescence in the 1.4-eV band of CdTe:In J. Appl. Phys. 110, 093103 (2011) Evidence of cation vacancy induced room temperature ferromagnetism in Li-N codoped ZnO thin films Appl. Phys. Lett. 99, 182503 (2011) Additional information on J. Appl. Phys. In this article we present size dependent spectroscopic observations of nanocolloids of ZnO. ZnO is reported to show two emission bands, an ultraviolet ͑UV͒ emission band and another in the green region. Apart from the known band gap 380 nm and impurity 530 nm emissions, we have found some peculiar features in the fluorescence spectra that are consistent with the nanoparticle size distribution. Results show that additional emissions at 420 and 490 nm are developed with particle size. The origin of the visible band emission is discussed. The mechanism of the luminescence suggests that UV luminescence of ZnO colloid is related to the transition from conduction band edge to valence band, and visible luminescence is caused by the transition from deep donor level to valence band due to oxygen vacancies and by the transition from conduction band to deep acceptor level due to impurities and defect states. A correlation analysis between the particle size and spectroscopic observations is also discussed.

Solid-immersion-lens-enhanced nonlinear frequency-variation mapping of a silicon integrated-circuit Appl. Phys. Lett. 99, 193103 (2011) A microfiber cavity with minimal-volume confinement Appl. Phys. Lett. 99, 051105 (2011) Lead silicate glass microsphere resonators with absorption-limited Q Appl. Phys. Lett. 98, 181105 (2011) Full band structure calculation of two-photon indirect absorption in bulk silicon Appl. Phys. Lett. 98, 131101 (2011) Geometry and quadratic nonlinearity of charge transfer complexes in solution: A theoretical study J. Chem. Phys. 134, 044534 (2011) Additional information on J. Appl. Phys. We have investigated the third-order nonlinearity in ZnO nanocolloids with particle sizes in the range 6-18 nm by the z-scan technique. The third-order optical susceptibility ͑3͒ increases with increasing particle size ͑R͒ within the range of our investigations. In the weak confinement regime, an R 2 dependence of ͑3͒ is obtained for ZnO nanocolloids. The optical limiting response is also studied against particle size.

In this paper, the fluorescence behaviour of nano colloids of ZnO has been studied as a function of the excitation wavelength. We have found that excitation at the tail of the absorption band gives rise to an emission that shifts with the change of the excitation wavelength. The excitation wavelength dependent shift of the fluorescence maximum is measured to be between 60 and 100 nm. This kind of excitation wavelength dependent fluorescence behaviour, which may appear to be in violation of Kasha's rule of excitation wavelength independence of the emission spectrum, has been observed for nano ZnO colloids prepared by two different chemical routes and different capping agents. It is shown that the existence of a distribution of energetically different molecules in the ground state coupled with a low rate of the excited state relaxation processes, namely, solvation and energy transfer, are responsible for the excitation wavelength dependent fluorescence behaviour of the systems.

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In this article, we present the spectral and nonlinear optical properties of ZnO–CdS nanocomposites prepared by colloidal chemical synthesis. The optical band gap (Eg) of the material is tunable between 2.62 and 3.84 eV. The emission peaks of ZnO–CdS nanocomposites change from 385 to 520 nm almost in proportion to changes in Eg. It is possible to obtain a desired luminescence color from UV to green by simply adjusting the composition. The nonlinear optical response of these samples is studied by using nanosecond laser pulses from a tunable laser at the excitonic resonance and off-resonance wavelengths. The nonlinear response is wavelength dependent, and switching from saturable absorption (SA) to reverse SA (RSA) has been observed for samples as the excitation wavelength changes from the excitonic resonance to off-resonance wavelengths. Such a changeover in the sign of the nonlinearity of ZnO–CdS nanocomposites is related to the interplay of exciton bleach and optical limiting mechanisms. The ZnO–CdS nanocomposites show self-defocusing nonlinearity and good nonlinear absorption behavior at off-resonant wavelengths. The nonlinear refractive index and the nonlinear absorption increase with increasing CdS volume fraction at 532 nm. The observed nonlinear absorption is attributed to two photon absorption followed by weak free carrier absorption. The enhancement of the third-order nonlinearity in the composites can be attributed to the concentration of exciton oscillator strength. This study is important in identifying the spectral range and composition over which the nonlinear material acts as a RSA based optical limiter. ZnO–CdS is a potential nanocomposite material for the tunable light emission and for the development of nonlinear optical devices with a relatively small limiting threshold.

The annealing effect on the spectral and nonlinear optical (NLO) characteristics of ZnO thin films deposited on quartz substrates by sol-gel process is investigated. As the annealing temperature increases from 300–1050 °C, there is a decrease in the band gap, which indicates the changes of the interface of ZnO. ZnO is reported to show two emission bands, an ultraviolet (UV) emission band and another in the green region. The intensity of the UV peak remains the same while the intensity of the visible peak increases with increase in annealing temperature. The role of oxygen in ZnO thin films during the annealing process is important to the change in optical properties. The mechanism of the luminescence suggests that UV luminescence of ZnO thin films is related to the transition from conduction band edge to valence band, and green luminescence is caused by the transition from deep donor level to valence band due to oxygen vacancies. The NLO response of these samples is studied using nanosecond laser pulses at off-resonance wavelengths. The nonlinear absorption coefficient increases from 2.9×10−6 to 1.0×10−4 m/W when the annealing temperature is increased from 300 to 1050 °C, mainly due to the enhancement of interfacial state and exciton oscillator strength. The third order optical susceptibility χ(3) increases with increase in annealing temperature (T) within the range of our investigations. In the weak confinement regime, T2.4 dependence of χ(3) is obtained for ZnO thin films. The role of annealing temperature on the optical limiting response is also studied.

In the present work, we report the third order nonlinear optical properties of ZnO thin films deposited using self assembly, sol gel process as well as pulsed laser ablation by z scan technique. ZnO thin films clearly exhibit a negative nonlinear index of refraction at 532 nm and the observed nonlinear refraction is attributed to two photon absorption followed by free carrier absorption. Although the absolute nonlinear values for these films are comparable, there is a change in the sign of the absorptive nonlinearity of the films. The films developed by dip coating and pulsed laser ablation exhibit reverse saturable absorption whereas the self assembled film exhibits saturable absorption. These different nonlinear characteristics in the self assembled films can be mainly attributed to the saturation of linear absorption of the ZnO defect states.

a b s t r a c tIn this Letter we present the spectral and nonlinear optical properties of ZnO-Ag nanocomposites prepared by colloidal chemical synthesis. Obvious enhancement of ultraviolet (UV) emission of the samples is observed and the strongest UV emission is over three times than that of pure ZnO. These nanocomposites show self-defocusing nonlinearity and good nonlinear absorption behaviour which increases with increasing Ag volume fraction. The observed nonlinear absorption is explained through two photon absorption followed by free carrier absorption. ZnO-Ag is a potential nanocomposite material for the UV light emission and for the development of nonlinear optical devices with a relatively small limiting threshold.