Multilayer Au/TiO2Composite Films with Ultrafast Third-Order Nonlinear Optical Properties

We report on the ultrafast third-order optical nonlinearity in multilayer Au/TiO2 composite films fabricated on quartz substrates by pulsed laser deposition technique. The linear optical properties of the films are determined and optical absorption peaks due to surface plasmon resonance of Au particles are observed at about 590hm. The third-order optical nonlinearities of the films are investigated by z-scan method using a femtosecond laser （50 fs） at the wavelength of 800 nm. The sample showed fast nonlinear optical responses with nonlinear absorption coefficient and nonlinear refractive index being -3.66 × 10^-10 m/W and -2.95 × 10^-17 m^2/W, respectively. The results also show that the nonlinear optical effects increase with the increasing Au concentration in the composite films.     

Nonlinear optical response of Au and Ag nanoparticles doped polyvinylpyrrolidone thin films

Colloidal Au and colloidal Ag were prepared by chemical reaction method and the nonlinear optical properties of Au and Ag nanoparticles doped polyvinylpyrrolidone (PVP) composite films were investigated using Z-scan technique with 38 ps pulses at 532 nm. Open aperture Z-scan measurements indicated that both the Au/PVP and Ag/PVP composite films exhibited reverse saturable absorption. Nonlinear absorption coefficients and third-order nonlinear refractive indices were determined. The mechanisms accounting for the process of nonlinear refractions were analyzed and the figures of merit W and T of the Au/PVP and Ag/PVP composite films were evaluated.     

Optical Nonlinear Properties of CdSeS/ZnS Core/Shell Quantum Dots

The optical nonlinear properties of CdSeS/ZnS quantum dots (QDs) areinvestigated by Z-scan technique using fundamental harmonic generation(1064nm) of mode-locked Nd:YAG laser for the first time. The experimental results show that two photon absorptions (TPA) occur at input intensity up to 12.5GW/cm². CdSeS/ZnS QDs have an average TPA cross section of 13710GM and large nonlinear refractive index on order of 10^-7esu. The large optical nonlinearities perhaps allow the CdSeS/ZnS QDs to be one kind of candidate material for bioimaging and fluorescence label, optical limiting and all-optical switching.     

Measurement of nonlinear properties and optical limiting ability of Rhodamine6G doped silica and polymeric samples

The third order nonlinear optical properties of Rhodamine6G (Rh6G) doped silica and polymeric samples have been investigated using single beam z-scan technique under excitation by the second harmonic of Nd:YAG laser beam (532 nm). The nonlinear refractive index, nonlinear absorption coefficient, real and imaginary parts of third order nonlinear susceptibility in the samples of silica and poly-methylmethacrylate (PMMA) matrices are measured. Thermal contribution to the nonlinear refractive index in case of undoped silica samples has been calculated in order to have better accuracy of the material response contribution to third order nonlinearity. The comparative study of the optical limiting performance of Rh6G doped silica and polymeric samples show that Rh6G doped silica is relatively superior for optical limiting applications.     

Nonlinear Optical Properties of Novel Polymeric Rare Earth Phthalocyanine Studied Using Picosecond Z-Scan Technique

Three novel tri-dimensional phthalocyanine polymers, with lanthanum （LaPPc）, gadolinium （GdPPc） and ytterbium （YbPPc） as centric atoms, have been synthesized from a tetranuclear phthalonitrile. Third-order optical nonlinearities of these compounds in DMF solution are measured by a picosecond Z-sacn technique at 532 nm. It is found that all the compounds show reverse saturation absorption and nonlinear self-focus refraction effect. The second-order molecular hyperpolarizabilities are calculated to be 1.82×10^-23, 1.48×10^-23 and 1.45×10^-23 esu for LaPPc, GdPPc and YbPPc, respectively. The differences among their nonlinear optical properties are attributed to the special tri-dimensional structure and the variation in rare earth atoms.     

Nonlinear optical and optical power limiting studies on a new thiophene-based conjugated polymer in solution and solid PMMA matrix

An experimental investigation of the third-order nonlinear optical properties of new poly{2-{5-[3,4-ditetradecyloxy-5-(1,3,4-oxadiazol-2-yl)thiophen-2-yl]-1,3,4-oxadiazol-2-yl}pyridine} (P) in tetrahydrofuran (THF) solution and in solid poly(methylmethacrylate) (PMMA) matrix, by Z-scan technique is reported. The Z-scan traces reveal that the composite films exhibit large negative nonlinear refractive index of the order 10⁻¹⁰ esu. The excited-state absorption cross-section was found to be larger than the ground-state absorption indicating that the operating nonlinear process is reverse saturable absorption (RSA). The new polymer P exhibits good optical power limiting properties in the nanosecond regime in solution and as well in solid PMMA matrix.     

Third-order nonlinear optical response of Au-core CdS-shell composite nanoparticles embedded in BaTiO<Subscript>3</Subscript> thin films

Au-core CdS-shell composite nanoparticles were synthesized by a direct self-assembly process and integrated into BaTiO₃ thin films. Characterization by transmission electron microscopy showed that the average diameter of these composite nanoparticles was about 8 nm. Using the femtosecond time-resolved optical Kerr effect method, we investigated the third-order nonlinear optical response of the Au@CdS nanoparticles embedded in the BaTiO₃ thin films at a wavelength of 800 nm. An ultrafast nonlinear response and a large effective third-order nonlinear susceptibility of χ⁽³⁾=7.7×10^-11 esu were observed. We attributed the enhancement of the third-order optical nonlinearity to a localized electric field effect originating from the core-shell structure under off-surface-plasmon resonance conditions. Received: 13 May 2002 / Revised version: 23 October 2002 / Published online: 3 April 2003 RID="*" ID="*"Corresponding author. Fax: +86-21/6510-4949, E-mail: sxqian@fudan.ac.cn     

Femtosecond Third-Order Optical Nonlinearity of Au：Bi203 Nanocomposite Films

Ultrafast third-order optical nonlinearities of the as-deposited and annealed Au：Bi2O3 nanocomposite films deposited by magnetron cosputtering are investigated by using femtosecond time-resolved optical Kerr effect （OKE） and pump probe techniques. The third-order optical nonlinear susceptibility is estimated to be 2.6Ф×10^- 10 esu and 1.8 × 10.9 esu at wavelength of 800nm, for the as-deposited and the annealed film, respectively. The OKE signal of the as-deposited film is nearly temporally symmetrical with a peak centred at zero delay time, which indicates the dominant contribution from intraband transition of conduction electrons. For the annealed film, the existence of a decay process in OKE signal implies the important contribution of hot electrons. These characteristics are in agreement with the hot electron dynamics observed in pump probe measurement.     

银/二氧化钛核壳纳米颗粒对碲化镉纳米晶的荧光增强研究

利用新合成的复合纳米结构银/二氧化钛核壳纳米颗粒,研究了金属银纳米颗粒对碲化镉纳米晶层荧光的增强情况.结果表明,这种新型复合金属纳米结构能极大地增强发光纳米晶层的荧光强度.银/二氧化钛核壳纳米颗粒是以水合肼、硝酸银和四异丙氧基钛为原材料,利用胶体化学法在水溶液中合成.透射电子显微镜图片表明这种新合成的银/二氧化钛纳米材料基本上呈球形,有较为明显的核壳结构,中间黑色的核是银纳米颗粒,外层颜色较浅部分是二氧化钛壳层.另外,包裹二氧化钛壳层后,银纳米颗粒的表面等离子吸收带从409 nm红移至430 nm,也证实了这种新型核壳纳米材料的形成.将此合成方法得到的银/二氧化钛纳米颗粒和碲化镉纳米晶用旋转涂覆方法进行直接组合后,得到了银纳米颗粒对碲化镉纳米晶荧光的明显增强,并对其增强的物理过程进行了讨论.这种能够增强荧光团发光的新型复合银纳米结构将在发光器件、荧光成像、生物探测等方面具有一定的应用价值.     

Annealing effect on the ultrafast dynamics of Ag nanoparticles embedded in soda-lime silicate glasses

Ag nanoparticles embedded in soda-lime silicate glasses were fabricated by the ion-exchange technique. Effects of thermal treatment on the optical nonlinearity and ultrafast dynamics of Ag nanoparticles were investigated by applying time-resolved optical Kerr effect and pump-probe techniques. The results indicate that thermal treatment is an efficient method to improve the nonlinear optical performance of this kind of material.     

Structural and Magnetic Properties of Fe-Doped Anatase TiO2 Films Annealed in Vacuum

Structural and magnetic properties of Fe-doped anatase TiO2 films fabricated by sol-gel spin coating are investigated. X-ray diffraction measurements reveal that Fe^3＋ ions are incorporated into the TiO2 lattice. No ferromagnetism-related secondary phases and magnetic nanopaxticles are observed in the films. The presence of electron paramagnetic resonance signals at 9- 2.0 supports oxygen vacancies and/or defects generated in the films after annealing in vacuum. Magnetic measurements indicate that Fe-doped anatase TiO2 films are ferromagnetic at room temperature. These observations suggest that oxygen vacancies and/or defects axe energetically favorable for the long range Fe^3＋-Fe^3＋ ferromagnetic coupling in Fe-doped anatase TiO2 films.     

Nonlinear optical properties of nanometer-size silver composite azobenzene containing polydiacetylene film

Diacetylene monomer containing p-nitrophenyl azobenzene moiety (NADA) was synthesized. Silver nanoparticles with different concentrations were adulterated in the above polymerized NADA (PNADA) films and the third-order nonlinear optical properties were investigated in detail. UV–vis spectra and transmission electron microscopy were used to confirm the formation of PNADA/Ag nanocomposite films. The silver nanoparticles (average size of 10 nm) were well dispersed in the polymer films. The value of the nonlinear refractive index n ₂ for PNADA films (8.48×10⁻¹⁵ cm²/W) was much higher than that of pure polydiacetylene films. Further, the introduction of silver nanoparticles into the PNADA polymer films led to the further enhancement of nonlinear optical properties. The maximum value of n ₂ for PNADA/Ag nanocomposite films could be 11.6×10⁻¹⁵ cm²/W. This enhancement should be ascribed to the surface plasmon resonance of silver nanoparticles.     

Two-photon absorption-induced optical properties of a new lasing dye in two solvents

Pumped by an infrared lasing and its frequency-doubling source, the fluorescence and superradiance emission properties of a new lasing dye trans-4-[4^′-(N,N-diethylamino)styryl]-N-methyl pyridinium methyl sulfate (abbreviated DEASPS), have been studied in benzyl alcohol and chloroform. The two-photon absorption (TPA) and emission properties of DEASPSare influenced by the solvents used. The emission wavelength of the dye in benzyl alcohol is redshifted relative to that in chloroform. The lifetime of two-photon absorption-induced fluorescence is about 529 ps in benzyl alcohol, whereas it is 340 ps in chloroform. Correspondingly, the one-photon-excited fluorescence lifetimes in the two solvents are also given. The upconversion efficiency of DEASPS in chloroform is higher than in benzyl alcohol. Finally, the effective molecular two-photon absorption cross-sections were measured by the nonlinear transmittance method. It is found that the optical limiting effect of the dye in benzyl alcohol is stronger than that in chloroform. Received: 3 May 2001 / Revised version: 6 July 2001 / Published online: 19 September 2001     

Large Third-Order Optical Nonlinearity of Cadmium Sulphide Nanoparticles Embedded in Polymer Thin Films

A simple method for synthesis of well dispersed cadmium sulphide nanoparticles embedded in a polyethylene glycol matrix （PEG 400） in thin film form is presented. The large blue shift of the band gap energy of the CdS nanoparticles compared to the bulk semiconductors is observed via UV-vis absorption spectra. Photoluminescence spectra of CdS nanocomposite films show that the emission peaks shift towards the longer wavelength with the increase of annealing temperature. Transmission electron microscopic images as well as Raman scattering studies confirm the CdS nanometer size particle formation within the polymer matrix. The particle size is about 8 nm. Selected area electron diffraction （SAED） shows the cubic zinc blende polycrystalline rings. Third-order optical nonlinearity of the CdS nanopartieles embedded in polymer thin films is studied with the Z-scan technique under 1064 nm excitation. The results show that the CdS nanocomposite film exhibits negative nonlinear refraction index and positive absorption coefficient. The film shows large optical nonlinearity, and the magnitude of the third-order nonlinear susceptibility of the film is calculated to be 1.73 × 10^-9 esu. The corresponding mechanism is discussed.     

SERS study of Ag nanoparticles electrodeposited on patterned TiO2 nanotube films

In this work, Ag nanoparticles (NPs) were deposited on patterned TiO₂ nanotube films through pulse‐current (PC) electrodeposition, and as a result patterned Ag NPs films were achieved. Scanning electron microscopy (SEM), electron probe microanalysis (EPMA), and X‐ray diffraction (XRD) were used, respectively, to study the morphology, uniformity, and phase structure of the patterned Ag NP films. The size and density of the as‐deposited Ag NPs could be controlled by changing the deposition charge density, and it was found that the patterned Ag NP films produced under a charge density of 2.0 C cm⁻² gave intense UV–vis and Raman peaks. Two‐dimensional surface‐enhanced Raman scattering (SERS) mapping of rhodamine 6G (R6G) on the patterned Ag NP films demonstrated a high‐throughput, localized molecular adsorption and micropatterned SERS effect. Copyright © 2010 John Wiley & Sons, Ltd.     

金/银纳米颗粒对Eu掺杂薄膜发光特性影响的研究

本文将三种金属纳米颗粒(球形银纳米颗粒、三角形银纳米薄片和三角形金纳米薄片)分别置于Eu(TTFA)3掺杂的Su8薄膜上研究了它们对铕配合物薄膜发光的影响.结果显示,金属纳米颗粒的局域等离子体共振(LSPR)谱对薄膜发光有很好的调控作用.对于LSPR谱分别与铕配合物激发谱和辐射谱重叠较好的球形和三角形两种银颗粒,相比于未放置颗粒时薄膜的发光,放置有颗粒的发光有明显的增强,其中球形银颗粒的样品的发光增强效果更为明显.而对于LSPR谱与铕配合物激发谱和辐射谱都不重叠的三角形片状金颗粒,该颗粒对样品的发光则起到了猝灭作用.     

Preparation and the optical nonlinearity of surface chemistry improved titania nanoparticles in poly(methyl methacrylate)-titania hybrid thin films

With 800-nm, 120-fs laser pulses, optical nonlinearity has been studied in a series of thin films containing poly(methyl methacrylate) (PMMA), filled with surfactant acetylacetone (Acac) capped TiO₂ nanoparticles, which were synthesized by a simple in situ sol-gel/polymerization process, assisted by spin coating and multi-step baking. The resulting nanohybrid thin films have highly optical transparency and demonstrate a unique nonlinear optical (NLO) response. The highest nonlinear refractive index (n₂) is observed up to 6.55 × 10⁻² cm² GW⁻¹ in the nanohybrid thin film of 60 wt% Ti(OBu)₄ in PMMA, with a negligible two-photon absorption (TPA), as confirmed by the Z-scan technique. The titanium precursor loading combined with the nature of the capping molecules are used to influence the ability of nanoparticles to nonlinear optical response. Indeed, the ligands at the nanoparticles’ surface can not only control the extent of the interaction between the organic molecules and the embedded nanoparticles but also influence the optical nonlinearities of nanoparticles.     

准波导结构下染料薄膜的荧光光谱和放大自发辐射光谱特性

通过对RhB/PMMA和Rh6G/PMMA染料薄膜的荧光光谱和放大自发辐射(ASE)光谱的实验测量和理论分析,研究了准波导结构染料薄膜的荧光光谱和ASE光谱特性。实验上采用连续激光和脉冲激光照射,分别测量准波导结构RhB/PMMA和Rh6G/PMMA染料薄膜的荧光光谱和ASE光谱,发现荧光峰和ASE峰随着染料掺杂浓度和薄膜厚度的增加产生红移;理论上考虑准波导结构下薄膜中染料的自吸收效应,类比激光器谐振腔模型,分析低阶导模传输的增益特性,获得了荧光光谱与ASE光谱中荧光峰和ASE峰对应波长与染料掺杂浓度的关系,数值计算与实验测量相吻合。结果表明,准波导结构下薄膜中染料自吸收效应导致荧光峰及ASE峰发生红移,改变染料掺杂浓度,可以在较大调谐范围实现ASE。     

密排银颗粒薄膜的制备及其SERS应用

银纳米颗粒通过自组装形成二维结构薄膜具有独特的光学性质,其提供的大量“热点”使其成为优越的表面增强拉曼散射(Surface enhanced Raman Scattering,SERS)基底.本文采用水/正己烷界面上自组装的方法得到了由密排的银纳米颗粒构成的薄膜,并以Rhodamine 6G为探针分子,比较了不同尺寸银...     

Significant modifications in the electrical properties of poly(methyl methacrylate) thin films upon dispersion of silver nanoparticles

Electrical conductivity of thin solid films of PMMA with dispersed silver nanoparticles, synthesized by a novel method, was studied in dark conditions by changing the applied voltage and temperature and also under photoexcitation (by a mercury lamp, 125 W) at room temperature. Anomalous hysteresis in current-temperature characteristics during heating and cooling cycles was observed. The hysteresis-like behaviour was explained on the basis of the movements of molecules associated with different parts of a PMMA matrix and diffusion of silver nanoparticles in the PMMA matrix. Dark current in the PMMA films with dispersed silver nanoparticles has been observed to be higher than the corresponding current in the PMMA films without silver nanoparticles due to the creation of conduction paths by the silver nanoparticles/nanoclusters. The photoresponse in the thin solid films of PMMA with dispersed silver nanoparticles was the reverse of that observed in thin solid films of PMMA without silver nanoparticles. A decrease in photocurrent under illumination of light was observed due to the destruction of conduction paths by the illumination of light.