Artificially nanostructured Cu:Al2O3 films produced by pulsed laser deposition

The processes leading to the formation of Cu:Al₂O₃ composite films on Si (001) with a well defined nanostructure by alternate pulsed laser deposition (a-PLD) in vacuum are investigated. Alternately amorphous Al₂O₃ layers and Cu nanocrystals nucleated on the Al₂O₃ surface are formed, according to the PLD sequence. The Al₂O₃ deposited on the Cu nanocrystals fills in the space between them until they are completely buried, and subsequently, a continuous dense layer with a very flat surface (within 1 nm) is developed. The nucleation process of the nanocrystals and their resulting oblate ellipsoidal shape are discussed in terms of the role of the energetic species involved in the PLD process and the metal–oxide interface energy. Received: 4 July 2000 / Accepted: 5 July 2000 / Published online: 13 September 2000     

Erasure effect of the reading beam on the decay process of χ(2) in all-optical poling

We have studied the effect of the reading beam on the decay process of the photoinduced second-order susceptibility χ⁽²⁾ in both the guest-host system (disperse red 1-doped polymethyl methactrylate) and the side-chain system (disperse red 19-functionalized polyimide polymer). Both experimentally and theoretically, we have proved that the reading beam has the erasure effect on the decay process, that is, χ⁽²⁾ decays faster in the high intensity than in the low intensity of the reading beam. Furthermore, the relationship between the time constant τ_B of the slow component of the decay process and the intensity of the reading beam I_1.06 is derived from the theoretical equations, which is fitted well with the experimental results. Based on the fitting parameters, we also compare, quantitatively, the thermal-induced orientational diffusion of trans- and the quantum efficiency of trans-to-cis photoisomerization in the two systems. Received: 8 September 1999 / Revised version: 14 March 2000 / Published online: 16 August 2000     

Theoretical analysis of optical properties of dielectric coatings dependence on substrate subsurface defects

A model for refractive index of stratified dielectric substrate was put forward according to theories of inhomogeneous coatings. The substrate was divided into surface layer, subsurface layer and bulk layer along the normal direction of its surface. Both the surface layer (separated into N₁ sublayers of uniform thickness) and subsurface layer (separated into N₂ sublayers of uniform thickness), whose refractive indices have different statistical distributions, are equivalent to inhomogeneous coatings, respectively. And theoretical deduction was carried out by employing characteristic matrix method of optical coatings. An example of mathematical calculation for optical properties of dielectric coatings had been presented. The computing results indicate that substrate subsurface defects can bring about additional bulk scattering and change propagation characteristic in thin film and substrate. Therefore, reflectance, reflective phase shift and phase difference of an assembly of coatings and substrate deviate from ideal conditions. The model will provide some beneficial theory directions for improving optical properties of dielectric coatings via substrate surface modification.     

Nonlinear optical properties of (B3O7)5- and (B3O6)3- groups

3 O₅ (LBO) crystal has been studied by using the bond valence theory of complex crystals. Chemical bond parameters and linear and nonlinear optical (NLO) properties of each type of constituent chemical bonds are quantitatively determined. Because of the different crystal structure characteristics of LBO from those of β-BaB₂O₄ (BBO), the two anionic groups, (B₃O₇)^5- in LBO and (B₃O₆)^3- in BBO, play different roles in contributions to their own total NLO tensor coefficients of LBO and BBO, respectively. By comparison, we find that planar (B₃O₆)^3- groups are the ideal structure model, leading to little cancellation of contributions of each kind of bond in these groups, and this gives us a useful guide to design new NLO materials in the future. Received: 24 January 1997/Accepted: 27 March 1997     

Stress effect and evidence of ferroelectric weakening in highly c-axis-oriented PbTiO3 thin films

3 were successfully grown on Pt-coated SrTiO₃ single-crystal substrates by metalorganic chemical vapor deposition (MOCVD) and were investigated by using X-ray diffraction (XRD), scanning electron microscopy (SEM) and Raman spectroscopy. The as-deposited thin films were found to be highly (001)-oriented with an average grain size of about 0.3 μm. Both a decrease of the tetragonality and a frequency downshift of the long-wavelength optical phonons were observed and attributed to the effect of compressive stress in the thin films. However, Raman scattering studies estimated a stress value of 2.6 GPa, which is much larger than the value of 0.75 GPa obtained from the XRD analyses. Raman spectroscopic studies also confirmed the grain-size-related disorder feature in the as-grown PbTiO₃ thin films. Structural investigations implied the weakening of ferroelectricity in the heteroepitaxial ferroelectric thin films. Received: 1 April 1997/Accepted: 14 July 1997     

Preparation and characterisation of compositionally graded BaxSr1-xTiO3 thin films

Ba_xSr_1-xTiO₃ thin films with a compositional gradient of x=0.3 to 1 (in 0.1 mole fraction increments) were fabricated on Pt/Ti/SiO₂/Si substrates using a modified sol–gel technique. The graded film crystallised in a perovskite structure and consists of a uniform microstructure with comparatively larger grains. The room-temperature relative dielectric constant (ε_r) and dielectric loss (cosδ) at 100 kHz were found to be 305 and 0.03 respectively. Dielectric peaks were not observed in the temperature range from -20 °C to 120 °C. The dielectric constant and dielectric loss were almost independent of temperature. Polarisation–electric field measurements at room temperature revealed a saturated but slim hysteresis loop with a remanent polarisation (P_r) of 0.6 μC/cm² and a coercive field (E_c) of 2.4 kV/mm. The graded film behaves as a stack of Ba_xSr_1-xTiO₃ capacitors connected in series and hence the dielectric Curie peaks are removed. Received: 4 October 2001 / Accepted: 17 October 2001 / Published online: 23 January 2002     

Optical poling in a crosslinkable polymer system

Received: 30 September 1998 / Published online: 24 February 1999     

First Z-scan n2 measurements on crystal hosts for ultraviolet laser systems

We report the results of the first measurements of the non-linear Kerr refractive index, n₂, for LiBaF₃ and LiLuF₄ crystal hosts, known as prospective UV-emitting tunable laser media when doped with Ce³⁺ ions. These n₂ values (2.7×10^-16 and 1.5×10^-16 cm²/W at 532 nm, respectively), obtained using the well-established Z-scan technique, are important for the characterization of new optical materials particularly in relation to their potential ultrafast applications. Received: 6 June 2000 / Published online: 5 October 2000     

Nonlinear phase shift without cascaded second-order processes and third-order nonlinearity

A new mechanism for obtaining a nonlinear phase shift has been proposed and schemes are described for its implementation. As it is shown, the interference of two waves with intensity-dependent amplitude ratio coming from the second-harmonic generation should produce the nonlinear phase shift. The sign and amount of nonlinear distortion of a beam wavefront is dependent on the relative phase of the waves that is introduced by the phase element. The calculated value of n₂ ^eff exceeds that connected with cascaded quadratic nonlinearity, at the same conditions. Received: 1 November 1999 / Published online: 23 February 2000     

Second-harmonic generation from a picosecond Ti:Sa laser in LBO: conversion efficiency and spatial properties

We report an experimental study of the second harmonic generated in type I interaction by a Ti:Sa laser operating in the picosecond regime at 786 nm in LBO crystals. A joint characterization of the dependence of conversion efficiency and spatial beam quality on crystal length and degree of pump focusing is given. A simple heuristic formula, reproducing over a broad range of parameters the predictions of classical Boyd–Kleinman theory, is derived and compared with the experimental results. The conditions for the optimization of the generation process using an elliptically focused pump beam are quantitatively evaluated. Received: 13 March 2002 / Revised version: 8 May 2002 / Published online: 12 July 2002     

Charge-separated-state enhancement of the third-order optical nonlinearity of a photosensitizer-electron acceptor triad assembly

′ ,4^′′,4^′′′-tetrasulfonato-phthalocyanine/N-butyl-N^′-methylanthraquinone-4,4^′-bipyridinum dibromide assembly (ZnTsPc-V-AQ), was observed to be enhanced by ten times when the sample was optically pumped by a 355 nm pump beam. The enhancement of the nonlinearity was found to be due predominantly to the charge transfer between the two monomers of the supramolecule after optical excitation. Received: 2 July 1996     

Analytical functions for the optimization of second-harmonic generation and parametric generation by focused Gaussian beams

An analytical function involving four parameters is proposed to express the second-harmonic generation efficiency as well as the parametric generation gain coefficient in the Boyd–Kleinman theory. The analytical function clearly reveals the dependence of conversion efficiency on the focusing parameter and the walk-off parameter. Moreover, the optimum focusing parameter and its corresponding maximum efficiency are explicitly given in the analytical function, leading to a straightforward evaluation of a given crystal performance. Received: 20 January 2003 / Published online: 22 May 2003 RID="*" ID="*"Corresponding author. Fax: +886-35/7291-34, E-mail: yfchen@cc.nctu.edu.tw     

Microstructures and dielectric properties of compositionally graded (Ba1-xSrx) TiO3 thin films prepared by pulsed laser deposition

Compositionally graded (Ba_1-xSr_x)TiO₃ (BST) (x:0.0∼0.25) thin films were grown on Pt (111)/TiO₂/SiO₂/Si (100) substrates using layer-by-layer pulsed laser deposition in the temperature range 550–650 °C. Both downgraded (Ba/Sr ratio varying from 100/0 at the bottom surface to 75/25 at the top surface) and upgraded (Ba/Sr ratio varying from 75/25 at the bottom surface to 100/0 at the top surface) BST films were prepared. Their microstructures were systematically studied by X-ray diffractometry and scanning electron microscopy. A grain morphology transition from large ‘rosettes’ (>0.30 μm) to small compact grains (70–110 nm) was observed in the downgraded BST films as the deposition temperature was increased from 550 to 650 °C. No such grain morphology transition was detected in the upgraded BST films. Dielectric measurements with metal electrodes revealed an enhanced dielectric behavior in the downgraded films. This enhancement is mainly attributed to the large compressive stress field built up near the interface between the downgraded film and substrate. Furthermore, the BaTiO₃ layer in the downgraded BST films not only serves as a bottom layer but also as an excellent seeding layer for enhancing the crystallization of the subsequent film layers in the downgraded films. Received: 10 December 2001 / Accepted: 12 March 2002 / Published online: 19 July 2002 RID="*" ID="*"Corresponding author. Fax: 86-25/359-5535, E-mail: xhzhu@public1.ptt.js.cn     

Chemical-bond analysis of the nonlinear optical properties of the borate crystals LiB3O5, CsLiB6O10, and CsB3O5

The second-order nonlinear optical properties of practical borate crystals, LiB₃O₅, CsLiB₆O₁₀, and CsB₃O₅, which all contain the identical basic structural unit [the (B₃O₇)^5- group], have been quantitatively studied from the chemical-bond viewpoint. Differences in the nonlinear optical properties among these three borate crystals arise from the contributions of the different cations, i.e., the different interaction between the cation and the (B₃O₇)^5- anionic group. The chemical-bond method quantitatively expresses this important difference. At the same time, the current calculation also shows that the B₃O₇ group is a very important crystallographic frame in the crystalline borate solids; it offers different cations an excellent coordination environment. Received: 20 February 2001 / Accepted: 14 June 2001 / Published online: 30 August 2001     

Deep UV laser induced fluorescence in fluoride thin films

Fluorescence experiments have been performed to study the interaction of 193-nm laser radiation with dielectric thin films of LaF₃, AlF₃, and MgF₂. Spectral- and time-resolved measurements reveal the presence of cerium in LaF₃ and the influence of hydrocarbons in MgF₂ and LaF₃. Virtually no fluorescence response is observable in the case of AlF₃. Supplementary measurements on multilayer stacks confirm the contribution of hydrocarbon and cerium emission in high-reflective UV mirrors upon ArF excimer laser irradiation. Energy density dependent measurements indicate a linear absorption process as the origin of UV laser induced fluorescence in LaF₃. Luminescence calculations are applied as a helpful tool in order to account for interference effects that are inherently to be found in the multilayer emission spectra. Received: 21 May 2002 / Accepted: 23 May 2002 / Published online: 10 September 2002 RID="*" ID="*"Corresponding author. Fax: +49-3641/807-601, E-mail: heber@iof.fraunhofer.de     

Deep UV laser induced luminescence in oxide thin films

Time-resolved luminescence experiments have been set up in order to study the interaction of 193-nm laser radiation with dielectric thin films. At room temperature, Al₂O₃ coatings show photoluminescence upon ArF excimer laser irradiation, with significant intensity contributions besides the known substrate emission. Time- and energy-resolved measurements indicate the presence of oxygen-defect centers in Al₂O₃ coatings, which suggests a strong single-photon interaction at 193 nm by F⁺ and F center absorption. Measurements on highly reflective thin-film stacks, consisting of quarter-wave Al₂O₃ and SiO₂ layers, indicate similar UV excitations, mainly from color centers of Al₂O₃. Received: 20 February 2002 / Accepted: 11 April 2002 / Published online: 5 July 2002     

Pulse-parameter dependence of the configuration characteristics of a micro-structure in fused SiO2 induced by femtosecond laser pulses

The fabrication of a micro-structures in fused SiO₂ by femtosecond laser pulses was studied in the range of pulse duration 150∼500 fs, pulse energy 60 nJ to ∼7 μJ and wavelengths 400 nm and 800 nm. The characteristics of the cross section of the micro-structure were explained with the multiphoton-ionization and avalanche-ionization processes in the femtosecond laser-induced breakdown. The characteristics of the longitudinal length of the micro-structure relating to the direct-focusing and self-action effects are also discussed. Received: 10 January 2001 / Accepted: 7 April 2001 / Published online: 23 May 2001     

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     

Physical mechanism of two-photon response in semi-insulating GaAs

The physical mechanism of two-photon response （TPR） in semi-insulating GaAs is studied. The measured photocurrent generated from the fabricated hemispherical GaAs sample responding to 1.3μm continuous wave laser shows a quadratic dependence on the coupled optical power and no saturation with the bias. The angular dependence of the photocurrent on the azimuth is in agreement with the anisotropy of double-frequency absorption （DFA） in GaAs single crystals. These results demonstrate DFA is the dominant mechanism of TPR in GaAs.     

Homodyne detection of second-harmonic generation as a probe of electric fields

Received: 16 December 1998