Nonlinear propagation of fs laser pulses in liquids and evolution of supercontinuum generation

Nonlinear propagation of fs laser pulses in liquids and the dynamic processes of filamentation such as self-focusing, intensity clamping, and evolution of white light production have been analyzed by using one- and two-photon fluorescence. The energy losses of laser pulses caused by multiphoton absorption and conical emission have been measured respectively by z-scan technique. Numerical simulations of fs laser propagation in water have been made to explain the evolution of white light production as well as the small-scale filaments in liquids we have observed by a nonlinear fluorescence technique. (c) 2005 Optical Society of America.

Nonlinear response and optical limiting in SrBi2Ta2O9 thin films

SrBi2Ta2O9 (SBT) thin films on quartz substrates were prepared by use of the pulsed-laser deposition technique. The nonlinear refractive indices, n(2), Of the SBT films were measured by use of z-scan techniques with picosecond pulses. Large negative nonlinear refractive indices of 3.84 and 3.58 cm(2)/GW were obtained for the wavelengths 532 nm and 1.064 mum, respectively. The two-photon absorption coefficient was determined to be 7.3 cm/GW for 532 nm. The limiting behavior of SBT thin film on a quartz substrate was investigated in an f/5 defocusing geometry by use of 38-ps-duration, 532-nm, 1.064-mum. laser excitation. (C) 2001 Optical Society of America.

散射中心型超分辨近场结构的非线性光学特性研究进展

超分辨近场结构(Super-RENS)技术是近年来发展起来的一种新型近场光存储技术，是目前最有实用化前景的纳米尺度近场超分辨技术之一。初步研究表明，其近场超分辨特性与非线性响应密切相关，研究其非线性光学特性对阐明物理机制、发展新的掩模材料和非线性光学应用都具有重要意义。对散射中心型超分辨近场结构非线性光学特性的最新研究进展进行了介绍和分析。

飞秒激光所致金纳米粒子析出的玻璃非线性吸收

依据Z-scan技术，使用波长532nm的纳秒脉冲，研究了通过聚焦的飞秒脉冲诱导并辅以热处理得到的金纳米粒子析出的玻璃的非线性吸收．观察到金纳米粒子析出的玻璃具有饱和吸收特性．根据局域场效应，对实验结果拟合，得到在接近表面等离子体共振激发情况下，金纳米粒子三阶极化率虚部分别为Imχm^(3)=5．7×10^-7esu．玻璃样品中金纳米粒子的非线性响应主要起源于热电子贡献。

Nanosecond nonlinear absorption in Au and Ag nanoparticles precipitated glasses induced by a femtosecond laser

We obtain Au and Ag nanoparticles precipitated in glasses by irradiation of focused femtosecond pulses, and investigate the nonlinear absorptions of the glasses by using Z-scan technique with ns pulses at 532 nm. We observe the saturable absorption behavior for An nanoparticles precipitated glasses and the reverse saturable ones for Ag ones. We also obtain, by fitting to the experimental results in the light of the local field effect near and away from the surface plasmon resonance, chi(m)((3)) = 4.5 x 10(-7) and 5.9 x 10(-8) esu for m the imaginary parts of the third-order susceptibilities for Au and Ag nanoparticles, respectively. The nonlinear response of Au nanoparticles in the glass samples arises mainly from the hot-electron contribution and the saturation of the interband transitions near the surface plasmon resonance, whereas that of Ag nanoparticles in the glass samples from the interband transitions. These show that the obtained glasses can be used as optoelectronic devices suiting for different demands. (c) 2005 Elsevier B.V. All rights reserved.

Preparation and optical properties of silicate glasses containing Pd nanoparticles

We report the space selective precipitation of Pd nanoparticles in Pd2+ -doped silicate glass by ultrashort laser pulses irradiation and further annealing. Absorption spectra, transmission electron microscopy, refractive index measurement and Z-scan technique demonstrated that metallic Pd nanoparticles were precipitated in the glass sample after irradiation by an 800-nm femtosecond laser and subsequent annealing at 600 degrees C. We discuss a refractive index change and nonlinear absorption that combines the precipitation of Pd nanoparticles. Crown Copyright (c) 2005 Published by Elsevier B.V. All rights reserved.

Interaction between the intrinsic second- and third-order optical fields in an Al0.53Ga0.47N/GaN heterostructure

We present an experimental demonstration of the interaction between the intrinsic second- and third-order optical fields in an Al0.53Ga0.47N/GaN heterostructure. The sample was deposited by metal-organic chemical vapor deposition on (0001) sapphire. The nonlinear optical coefficients of the sample, which were measured with a Mach-Zehnder interferometer system, quadratically increase with the applied modulating voltage, indicating the existence of the third-order optical field. The third-order signal was then detected by the Z-scan method and we calculated the built-in dc field on the AlGaN/GaN interface to confirm the strong interaction between the intrinsic second- and third-order optical fields. (c) 2008 American Institute of Physics.

Third-order optical nonlinearities of lead-free (Na1-xKx)(0.5)Bi0.5TiO3 thin films

(Na1-xKx)(0.5)Bi0.5TiO3 (NKBT) (x = 0.1, 0.2, and 0.3) thin films with good surface morphology and rhombohedral perovskite structure were fabricated on quartz substrates by a sol-gel process. The fundamental optical constants (the band gaps, linear refractive indices and absorption coefficients) of the films were obtained through optical transmittance measurements. The nonlinear optical properties were investigated by Z-scan technique performed at 532 nm with a picosecond laser. A two-photon absorption effect closely related with potassium-doping content was found in thin films, and the nonlinear refractive index n(2) increases evidently with potassium-doping. The real part of the third-order nonlinear susceptibility chi((3)) is much larger than its imaginary part, indicating that the third-order optical nonlinear response of the NKBT films is dominated by the optical nonlinear refractive behavior. These results show that NKBT thin films have potential applications in nonlinear optics. (C) 2007 Elsevier B.V. All rights reserved.

Preparation and nonlinear optical properties of ultrathin composite films containing both a polyoxometalate anion and a binuclear phthalocyanine

An ultrathin composite film containing both polyoxometalate anion [PMo12O40](3-) ( PMo12) and a planar binuclear phthalocyanine, bi-CoPc, has been prepared by the electrostatic layer-by-layer self-assembly method. UV-vis measurements revealed regular film growth with each four-layer {PMo12/bi-CoPc/PSS/PAH} adsorption. The lm structure was characterized by small-angle X-ray reflectivity measurements, X-ray photoelectron spectra, and AFM images. The nanothick film shows a third-order nonlinear optical response of chi((3)) = 4.21 x 10(-12) esu. Experimental investigations also indicate that the combination of polyoxometalate anions [PMo12O40](3-) with the phthalocyanine bi-CoPc in multilayer films can enhance the third-order NLO susceptibility and modify the third-order NLO absorption of bi-CoPc.

Experimental measurement of polyethylene chain modulus by scanning force microscopy

Nanoindentation technique and scanning force microscopy have been used to measure directly the polyethylene modulus along the chain axis. Single crystals of polyethylene were employed in order to obtain well-aligned chain segments. To minimize effects of scanner creep, a Z scan rate of 3 Hz was employed. The "X Rotate" value of 25 degrees was selected to eliminate effects of lateral tip motion. The results were analyzed by the Oliver -Pharr method for which direct observation and measurement of the contact area are not required. Considering the influence of tip roundness on the projected contact area, the nanoindentation results were analyzed by the Sawa method. The chain modulus obtained from the thinner polyethylene single crystal sample was 204 +/- 21 GPa by the Oliver-Pharr method and 168 +/- 17 GPa by the Sawa method. The lower values than expected were due to substrate effects and anisotropy of chain deformation during nanoindentation. An extrapolation of the chain modulus obtained by various strains to zero nanoindentation eliminated the effect of substrate and anisotropy of chain deformation. The corresponding chain modulus obtained from the thicker sample was 278 GPa by the Oliver-Pharr method and 267 GPa by the Sawa method, respectively, in better agreement with the value of 340 Cpa determined theoretically. (C) 2001 Elsevier Science Ltd. All rights reserved.

Studies on two coordination polymers [M(mu(4)-pz25dc)](n) (M = Cd or Zn, pz25dc=pyrazine-2,5-dicarboxylato) with three-dimensional pillared-layer three-nodal framework: Synthesis, structural characterization, strong optical non-linearities and optical limiting properties

Two isomorphous new candidates [M(mu(4)-pz25dc)](n) (M = Cd, 1; Zn, 2; pz25dc = pyrazine-2,5-dicarboxylato)for nonlinear optical (NLO) materials have been synthesized hydrothermally and characterized crystallographically as pillared-layer three-nodal frameworks with one four-connected metal nodes and two crystallographically different four-connected ligand nodes. Their optical non-linearities are measured by the Z-Scan technique with an 8 ns pulsed laser at 532 nm. These two coordination polymers both exhibit strong NLO absorptive abilities [alpha(2) = (63 +/- 6) x 10 (12) mW (1) 1, ( 46 +/- 6) x 10 (11) mW (1) 2] and effective self-focusing performance [n(2) = (67 +/- 5) x 10 (18) 1, (13 +/- 3) x 10 (18) m(2) W (1) 2] in 1.02 x 10 (4) 1 and 1.05 x 10 (4) mol dm (3) 2 DMF solution separately. The values of the limiting threshold are also measured from the optical limiting experimental data. The heavy atom effect plays important role in the enhancement of optical non-linearities and optical limiting properties. (C) 2009 Elsevier B. V. All rights reserved.

Measurements of nonlinear refractive index in scattering media.

We have recently developed a spectral re-shaping technique to simultaneously measure nonlinear refractive index and nonlinear absorption. In this technique, the information about the nonlinearities is encoded in the frequency domain, rather than in the spatial domain as in the conventional Z-scan method. Here we show that frequency encoding is much more robust with respect to scattering. We compare spectral re-shaping and Z-scan measurements in a highly scattering environment and show that reliable spectral re-shaping measurements can be performed even in a regime that precludes standard Z-scans.

Reconstruction of atomic ionization probabilities in intense laser fields

Application of a parallel-projection inversion technique to z-scan spectra of multiply charged xenon and krypton ions, obtained by non-resonant field ionization of neutral targets, has for the first time permitted the direct observation of intensity-dependent ionization probabilities. These ionization efficiency curves have highlighted the presence of structure in the tunnelling regime, previously unobserved under full-volume techniques.

Plasma Polymerised Organic Thin Films-A Study on the Structural, Electrical and Nonlinear Optical Properties for Possible Applications

This proposed thesis is entitled “Plasma Polymerised Organic Thin Films: A study on the Structural, Electrical, and Nonlinear Optical Properties for Possible Applications. Polymers and polymer based materials find enormous applications in the realm of electronics and optoelectronics. They are employed as both active and passive components in making various devices. Enormous research activities are going on in this area for the last three decades or so, and many useful contributions are made quite accidentally. Conducting polymers is such a discovery, and eversince the discovery of conducting polyacetylene, a new branch of science itself has emerged in the form of synthetic metals. Conducting polymers are useful materials for many applications like polymer displays, high density data storage, polymer FETs, polymer LEDs, photo voltaic devices and electrochemical cells. With the emergence of molecular electronics and its potential in finding useful applications, organic thin films are receiving an unusual attention by scientists and engineers alike. This is evident from the vast literature pertaining to this field appearing in various journals. Recently, computer aided design of organic molecules have added further impetus to the ongoing research activities in this area. Polymers, especially, conducting polymers can be prepared both in the bulk and in the thinfilm form. However, many applications necessitate that they are grown in the thin film form either as free standing or on appropriate substrates. As far as their bulk counterparts are concerned, they can be prepared by various polymerisation techniques such as chemical routes and electrochemical means. A survey of the literature reveals that polymers like polyaniline, polypyrrole, polythiophene, have been investigated with a view to studying their structural electrical and optical properties. Among the various alternate techniques employed for the preparation of polymer thin films, the method of plasma polymerisation needs special attention in this context. The technique of plasma polymerisation is an inexpensive method and often requires very less infra structure. This method includes the employment of ac, rf, dc, microwave and pulsed sources. They produce pinhole free homogeneous films on appropriate substrates under controlled conditions. In conventional plasma polymerisation set up, the monomer is fed into an evacuated chamber and an ac/rf/dc/ w/pulsed discharge is created which enables the monomer species to dissociate, leading to the formation of polymer thin films. However, it has been found that the structure and hence the properties exhibited by plasma polymerized thin films are quite different from that of their counterparts produced by other thin film preparation techniques such as electrochemical deposition or spin coating. The properties of these thin films can be tuned only if the interrelationship between the structure and other properties are understood from a fundamental point of view. So very often, a through evaluation of the various properties is a pre-requisite for tailoring the properties of the thin films for applications. It has been found that conjugation is a necessary condition for enhancing the conductivity of polymer thin films. RF technique of plasma polymerisation is an excellent tool to induce conjugation and this modifies the electrical properties too. Both oxidative and reductive doping can be employed to modify the electrical properties of the polymer thin films for various applications. This is where organic thin films based on polymers scored over inorganic thin films, where in large area devices can be fabricated with organic semiconductors which is difficult to achieve by inorganic materials. For such applications, a variety of polymers have been synthesized such as polyaniline, polythiophene, polypyrrole etc. There are newer polymers added to this family every now and then. There are many virgin areas where plasma polymers are yet to make a foray namely low-k dielectrics or as potential nonlinear optical materials such as optical limiters. There are also many materials which are not been prepared by the method of plasma polymerisation. Some of the materials which are not been dealt with are phenyl hydrazine and tea tree oil. The advantage of employing organic extracts like tea tree oil monomers as precursors for making plasma polymers is that there can be value addition to the already existing uses and possibility exists in converting them to electronic grade materials, especially semiconductors and optically active materials for photonic applications. One of the major motivations of this study is to synthesize plasma polymer thin films based on aniline, phenyl hydrazine, pyrrole, tea tree oil and eucalyptus oil by employing both rf and ac plasma polymerisation techniques. This will be carried out with the objective of growing thin films on various substrates such as glass, quartz and indium tin oxide (ITO) coated glass. There are various properties namely structural, electrical, dielectric permittivity, nonlinear optical properties which are to be evaluated to establish the relationship with the structure and the other properties. Special emphasis will be laid in evaluating the optical parameters like refractive index (n), extinction coefficient (k), the real and imaginary components of dielectric constant and the optical transition energies of the polymer thin films from the spectroscopic ellipsometric studies. Apart from evaluating these physical constants, it is also possible to predict whether a material exhibit nonlinear optical properties by ellipsometric investigations. So further studies using open aperture z-scan technique in order to evaluate the nonlinear optical properties of a few selected samples which are potential nonlinear optical materials is another objective of the present study. It will be another endeavour to offer an appropriate explanation for the nonlinear optical properties displayed by these films. Doping of plasma polymers is found to modify both the electrical conductivity and optical properties. Iodine is found to modify the properties of the polymer thin films. However insitu iodine doping is tricky and the film often looses its stability because of the escape of iodine. An appropriate insitu technique of doping will be developed to dope iodine in to the plasma polymerized thin films. Doping of polymer thin films with iodine results in improved and modified optical and electrical properties. However it requires tools like FTIR and UV-Vis-NIR spectroscopy to elucidate the structural and optical modifications imparted to the polymer films. This will be attempted here to establish the role of iodine in the modification of the properties exhibited by the films

The tautomerism, solvatochromism and non-linear optical properties of fluorescent 3-hydroxyquinoxaline-2-carboxalidine-4-aminoantipyrine

The Schiff base, 3-hydroxyquinoxaline-2-carboxalidine-4-aminoantipyrine, was synthesized by the condensation of 3-hydroxyquinoxaline-2-carboxaldehyde with 4-aminoantipyrine. HPLC, FT-IR and NMR spectral data revealed that the compound exists predominantly in the amide tautomeric form and exhibits both absorption and fluorescence solvatochromism, large stokes shift, two electron quasireversible redox behaviour and good thermal stability, with a glass transition temperature of 104oC. The third-order non-linear optical character was studied using open aperture Z-scan methodology employing 7 ns pulses at 532 nm. The third-order non-linear absorption coefficient, b, was 1.48 x 10-6 cm W-1 and the imaginary part of the third-order non-linear optical susceptibility, Im c(3), was 3.36 x10-10 esu. The optical limiting threshold for the compound was found to be 340 MW cm-2.