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     

Laser-induced sign reversal of the nonlinear refractive index of Ag nanoclusters in soda-lime glass

Received: 16 February 1998     

Determination of nonlinear absorption and refraction by single Z-scan method

We report a simplified Z-scan technique based on a study on the symmetric features of a typical Z-scan curve. The contributions from the two-photon absorption (TPA) and the nonlinear refraction (NLR) are easily separated from a closed-aperture Z-scan curve using this method. And the determination of the two nonlinearities is simplified and unambiguous. We demonstrate this method on ZnSe, CdS, and ZnTe semiconductors with 120-fs laser pulses. And the influence from the uncertainty of the focal plane (Z=0) position is discussed. It is also found that the TPA coefficient can be obtained independently without knowing the exact location of the focal point. Received: 8 July 1999 / Published online: 3 November 1999     

Optical limiting in cobalt-doped polyvinylpyrrolidone

The results of optical limiting investigations of cobalt-doped polyvinylpyrrolidone solutions are presented. The optical limiting studies have shown that this process is due to self-defocusing at the wavelength of 1064 nm and also due to reverse saturable absorption and self-defocusing at the wavelength of 532 nm. The results of measurements on the non-linear optical characteristics of organometallic complexes are presented. Received: 10 July 2001 / Revised version: 15 October 2001 / Published online: 29 November 2001     

Random laser action in ZnO

We report a direct evidence of random laser in optically pumped ZnO powder. Discrete lasing modes are observed above threshold. The laser emission spectra depend on the angle of observation and are random. The lasing action is attributed to the coherent feedback due to recurrent light scattering in the powder. The lasing threshold intensity depends on the excitation volume. Received: 15 September 1999 / Revised version: 2 February 2000 / Published online: 5 July 2000     

Nonlinear change in refractive index of Co2+:ZnSe at short-pulse single-beam 1.54-μm Z-scan probing

An experimental study and theoretical modeling of the nonlinear change in refractive index of a Co^{2 +}: ZnSe crystal at the short-pulse single-beam probing at the wavelength 1.54 μm is reported. In the experimental conditions of negligible contributions in the index non-linearity stemming from the Kerr-effect and inhomogeneous heating, the nonlinear change in refractive index in Co^{2 +}:ZnSe is shown to be caused by the resonant Co^{2 +} population-perturbation effect (i.e., by the Co^{2 +} ground-state absorption saturation). The Z-scan single-beam technique and novel theoretical approach addressing the resonant nonlinear refraction in a saturable doped medium are used, respectively, for an experimental and theoretical inspection of the phenomenon. For a set of Co^{2 +}:ZnSe samples with different concentrations of Co^{2 +} ions at the short-pulse (200 ns) mJ-range probing, we show that the maximal nonlinear change in refractive index is about of units of 10^{− 4} at the chosen wavelength.     

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     

Efficient and compact intracavity-frequency-doubled Nd:GdVO4/KTP laser end-pumped by a fiber-coupled laser diode

A compact and efficient diode-pumped intracavity-frequency-doubled Nd:GdVO₄/KTP green laser is demonstrated with a flat–flat cavity design. With a 1.3 at. % Nd³⁺-doped GdVO₄ crystal and pumped at the weak-absorption peak of 806 nm, the second-harmonic output power at 532 nm was measured to be 1.95 W at an incident pump power of 8.4 W, corresponding to an optical conversion efficiency of 23.2%. The output characteristic at the fundamental wavelength of 1.063 μm was investigated with two different pump wavelengths. More than 4.5-W output power was generated when the laser was pumped at 806.2 nm. Received: 26 July 2000 / Revised version: 18 September 2000 / Published online: 7 February 2001     

Nonlinear optical response of Ge nanocrystals in silica matrix with excitation of femtosecond pulses

We report an investigation of third-order optical nonlinearities in Ge nanocrystals (∼6 nm radius) embedded in silica matrix using the Z-scan and pump-probe techniques with femtosecond laser pulses at 780-nm wavelength. The nanocrystallite Ge samples were prepared using magnetron co-sputtering and post-thermal annealing at 800 °C. The nonlinear absorption coefficient and refractive index of the Ge nanocrystals were determined to be in the range from 1.8×10^-7 to 6.8×10^-7 cm/W and 1.5×10^-12 to 8.0×10^-12 cm²/W, respectively, which are proportional to the Ge atomic fraction in the matrix. Relaxation of the nonlinear response was found to have two characteristic time constants, 1.8 ps and 65 ps. The mechanisms responsible for the observed nonlinear response are discussed. Received: 21 August 2000 / Revised version: 17 January 2001 / Published online: 30 March 2001     

Characterization of nonlinear optical parameters of polymethine dyes

We investigated nonlinear refraction, nonlinear absorption, and saturable absorption of polymethine dyes by the Z-scan technique (λ=1064 nm). The analysis of simultaneous appearance of several nonlinear optical processes in dye solutions excited by picosecond pulses was carried out. The saturable absorption was analyzed taking into account various models. Nonlinear refractive indices, nonlinear absorption coefficients, and saturation intensities of various polymethine dyes were measured. Received: 27 December 2002 / Revised version: 6 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-471/363-366, E-mail: r_ganeev@issp.u-tokyo.ac.jp RID="**" ID="**"Present address: The Institute for Solid State Physics, The Tokyo University, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan     

Visible and infrared dispersion of the refractive indices in periodically poled and single domain Nd:Mg:LiNbO3 crystals

3 crystals are measured in the transparency region (with the accuracy ±0.0002) and for the upper phonon polariton branch (with the accuracy ±0.003–±0.05), from 0.44 μm up to 10.5 μm. The method of spontaneous parametric light scattering is used for measurement of the ordinary refractive index dispersion in the mid-infrared region and for determination of the domain grating period d=5.6±0.2 μm in the periodically-poled crystal. Received: 29 January 1997/Revised version: 10 July 1997     

Luminescence properties of thin films prepared by laser ablation of Nd-doped potassium gadolinium tungstate

Optically active thin films on Si substrates have been produced by laser ablation of a Nd-doped potassium gadolinium tungstate (Nd:KGW) single crystal. Films grown at low oxygen pressures (<0.6 mbar) are potassium-deficient and appear to be mainly disordered. They show a poor photoluminescence (PL) performance that improves upon annealing in air at temperatures in the range 700–1000 °C. Films grown at high oxygen pressure (1 mbar) show instead good stoichiometry and the presence of a dominant textured gadolinium-tungstate phase compared to KGW. These films have low absorption, a refractive index close to that of bulk KGW and good PL performance, the emission lifetimes being longer (τ>150 μs) under certain conditions than those measured in the single-crystal material. Received: 25 July 2001 / Accepted: 26 July 2001 / Published online: 17 October 2001     

Characterization of optical and nonlinear properties of periodically-poled RbTiOAsO4 in the mid-infrared range via difference-frequency generation

Tunable mid-infrared coherent radiation (3.25- 3.7 μm) is generated by quasi-phase-matched difference frequency generation in a multi-grating periodically-poled RbTiOAsO₄ crystal. The spontaneous polarization and coercive field of flux-grown RbTiOAsO₄ are determined by polarization switching measurements. The nonlinear interaction enables us to explore the optical and nonlinear properties of this material in the mid-infrared range, where data is scarce. The measurements are used to derive a mid- infrared corrected dispersion equation for n_z in RbTiOAsO₄. This equation is in excellent agreement with previously published measurements of nonlinear interactions in periodically-poled RbTiOAsO₄. The measured wavelength and temperature bandwidths are ≈48 nm cm and ≈29 °C cm, respectively. A relatively high temperature tuning slope of the phase-matched idler wavelength, -1.27 nm/°C, is measured. This may be useful for realizing temperature-tuned nonlinear devices. Received: 30 March 2000 / Revised version: 9 May 2000 / Published online: 30 June 2000     

Studies of third-order nonlinear optical properties of C60 by the optical Kerr effect

60 at 1.064 μm is determined by the optical Kerr effect in toluene solution. Values of -6.5×10^-33 esu and 2.0×10^-32 esu for the real and imaginary parts of γ, respectively, are obtained. Based on the experimental results and symmetry constraint, it is concluded that a three-level model is not adequate to describe the third-order nonlinearity of C₆₀. It is also inferred that the non-resonant γ of C₆₀ should be positive in sign, which is in agreement with reported off-resonant measurements of γ of C₆₀ by third-harmonic generation. Received: 3 September 1997/Revised version: 1 December 1997     

Optical nonlinearity enhancement for an anisotropic semiconductor–insulator composite

We investigate the effect of geometric anisotropy on the optical nonlinearity enhancement for a periodic composite with a rectangular array of elliptic semiconducting cylinders in an insulating host. By using a series expression of the space-dependent electric field obtained by a simple Fourier method in a periodic composite, we calculate the frequency dependence of the effective third-order nonlinear susceptibility as a function of anisotropy. The results show that the height of the nonlinearity enhancement peak may be increased by several orders of magnitude as the aspect ratio of the ellises is decreased or the lattice edge length ratio is increased. At resonance frequency, there exists a strong anomalous dispersion. We also investigate the effect of the volume fraction of the semiconductor phase for composites with a square array of circular semiconducting cylinders. Received: 23 November 2000 / Accepted: 2 August 2001 / Published online: 17 October 2001     

Fullerene-doped porous glasses

60 in porous glass by diffusion in solution phase at room temperature. The presence of C₆₀ in the doped porous glass was confirmed spectroscopically. We also report the changes in optical absorption spectrum and intensity-dependent transmission of 30 ns laser pulses at 527 nm in these materials. Received: 17 October 1996/Accepted: 27 February 1997     

Model for multiwave-pumped parametric oscillation in BaTiO3

3 crystal subjected to two counterpropagating pairs of pump beams. The model explains the characteristic features of the above effect and predicts a number of new peculiarities that we have found in additional experiments. Received: 19 March 1997/Revised version: 9 June 1997     

Measurement of the temperature dependence of quartz refractive indices

We present and discuss a technique to measure concurrently the temperature dependence of quartz refractive indices in the thermal range 25–300° C. The magnitude of both indices is found to decrease slightly with increasing temperature in the thermal range considered.     

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     

Structural and optical characterization of Er3+/Yb3+-doped LiNbO3

We report the dependence of the unit-cell parameters and the extraordinary and ordinary refractive indices of Er³⁺/Yb³⁺-codoped LiNbO₃ crystals. Both properties depend in a non-monotonic manner on the Er³⁺/Yb³⁺ content. A singularity was observed at concentrations of 1.1-1.2 mol. % in the crystal (0.6-0.7 mol. % in the melt). In the same way the Er and Yb concentration influences the periodically poled lithium niobate formation. The observed behavior of refractive indices and unit-cell parameters of Er³⁺/Yb³⁺-codoped LiNbO₃ crystals could be explained in terms of the RE³⁺-ion concentration affecting the Li-vacancy concentration and the RE³⁺-ion positions in the crystal. Received: 21 May 2001 / Revised version: 22 August 2001 / Published online: 23 October 2001