Ultrashort laser induced spatial redistribution of silver species and nano-patterning of etching selectivity in silver-containing glasses.

Femtosecond laser-induced spatial redistribution of silver species (ions, clusters, and hole centers) in a silver-containing phosphate glass is investigated by correlative means of near-field scanning optical microscopy (NSOM) images, numerical simulations, chemical micro-probe analysis, and nanoscale spatial profiles after soft etching. In particular, we found that the chemical etching selectivity for nanoscale patterning is strongly dependent upon the irradiation of femtosecond laser due to the spatial redistribution of silver species within the affected area. These results strongly indicate that controlling the distribution of silver species by femtosecond laser irradiation may open new routes for surface nanoscale chemical and/or spatial patterning for the fabrication of 2D surface photonic crystals.

Laser writing of nonlinear optical properties in silver-doped phosphate glass.

The formation of both local second- and third-harmonic generations (SHG and THG) induced by a train of femtosecond laser pulses in silver-doped phosphate glasses is addressed. Based on modeling calculations, including various diffusion and kinetic processes, THG is shown to result from the formation of silver clusters. The latter organize into a ring-shape structure, leading to the emergence of a static electric field. By breaking the glass centro-symmetry, this field gives rise to a local effective second-order susceptibility, inducing SHG. Both theoretically predicted SHG and THG evolutions with respect to the number of pulses in the train are in good agreement with experimental observations. In particular, the observed reaching of a maximum in the nonlinear optical responses after a few thousands of pulses is explained by the competition of various physical processes. A cooling of the glass is shown to improve the process efficiency of the laser writing of second-order nonlinearity.

Two-photon excited fluorescence in the LYB:Eu monoclinic crystal: towards a new scheme of single-beam dual-voxel direct laser writing in crystals.

We report on two-photon excited fluorescence in the oriented Eu(3+)doped LYB monoclinic crystal under femtosecond laser tight focusing. Due to spatial walk-off, the two polarization modes of the incident femtosecond beam simultaneously provide the independent excitation of two distinct focuses, leading to a single-beam dual-voxel nonlinear excitation of fluorescence below material modification threshold. These observations emphasize on the anisotropy of both two-photon absorption as well as fluorescence emission. They demonstrate the localized control of the nonlinear energy deposit, thanks to the adjustment of both the input power and polarization, by properly balancing the injected energy in each voxel. Such approach should be considered for future direct laser writing of waveguides in propagation directions out of the dielectric axes, so as to optimally cope with the highly probable anisotropy of laser-induced material modification thresholds in these crystals. These results open new ways for further potential developments in direct laser writing as the simultaneous inscription of double-line structures for original waveguides processes.

Propagation beam consideration for 3D THz computed tomography.

In this paper, a model of the beam propagation is developed according to the physical properties of THz waves used in THz computed tomography (CT) scan imaging. This model is first included in an acquisition simulator to observe and estimate the impact of the Gaussian beam intensity profile on the projection sets. Second, the model is introduced in several inversion methods as a convolution filter to perform efficient tomographic reconstructions of simulated and real acquired objects. Results obtained with three reconstruction methods (BFP, SART and OSEM) are compared to the techniques proposed in this paper. We will demonstrate an increase of the overall quality and accuracy of the 3D reconstructions.

Qualitative and quantitative investigation of chromium-polluted soils by laser-induced breakdown spectroscopy combined with neural networks analysis.

Laser-induced breakdown spectroscopy (LIBS) has been applied to the analysis of three chromium-doped soils. Two chemometric techniques, principal components analysis (PCA) and neural networks analysis (NNA), were used to discriminate the soils on the basis of their LIBS spectra. An excellent rate of correct classification was achieved and a better ability of neural networks to cope with real-world, noisy spectra was demonstrated. Neural networks were then used for measuring chromium concentration in one of the soils. We performed a detailed optimization of the inputs of the network so as to improve its predictive performances and we studied the effect of the presence of matrix-specific information in the inputs examined. Finally the inputs of the network--the spectral intensities--were replaced by the line areas. This provided the best results with a prediction accuracy and precision of about 5% in the determination of chromium concentration and a significant reduction of the data, too.

Laser-induced breakdown spectroscopy of composite samples: comparison of advanced chemometrics methods.

Laser-induced breakdown spectroscopy is used to measure chromium concentration in soil samples. A comparison is carried out between the calibration curve method and two chemometrics techniques: partial least-squares regression and neural networks. The three quantitative techniques are evaluated in terms of prediction accuracy, prediction precision, and limit of detection. The influence of several parameters specific to each method is studied in detail, as well as the effect of different pretreatments of the spectra. Neural networks are shown to correctly model nonlinear effects due to self-absorption in the plasma and to provide the best results. Subsequently, principal components analysis is used for classifying spectra from two different soils. Then simultaneous prediction of chromium concentration in the two matrixes is successfully performed through partial least-squares regression and neural networks.

Nondestructive analysis of the transverse structure of novel optical fibers by third-harmonic-generation microscopy.

We demonstrate the suitability of the third-harmonic-generation technique as a new nonlinear microprobe for nondestructive determination of the index profile of optical fibers. Photonic bandgap (Bragg-type) and air-silica microstructure (ASM) fibers were tested. The complete spatial characteristics, such as hole diameter and spacing into ASM fibers or sandwiched layer thickness into Bragg fibers, were demonstrated to be attainable anywhere along a bare fiber.

Nonlinearity measurements of thin films by third-harmonic-generation microscopy.

We show that the electronic part of the nonlinear susceptibility chi(3) of thin films can be easily measured by third harmonic microscopy. The phenomenon of third harmonic generation (THG) is excited by a femtosecond laser beam focused at the interface between the thin film and a reference layer. The value of chi(3) is deduced from the THG intensity measurements with the help of a classical model. The validity of this simple and alternative method is established by testing reference liquid films.

Imaging of Ca(2)+ intracellular dynamics with a third-harmonic generation microscope.

We describe the promising development of third-harmonic generation (THG) in laser scanning microscopy for study of the functional imaging of live biological cells. The dynamics of Ca(2+) in biological cells is shown. The Ca(2+) signal consists of a transient increase in the intracellular concentration. THG microscopy allows one to temporally visualize the release of Ca(2+) from internal stores and (or) calcium influx.

Coherent broadband pulse shaping in the mid infrared.

We demonstrate broadband infrared pulse shaping by difference-frequency mixing of two visible phase-locked linearly chirped pulses in GaAs. Control of the temporal profile of the emitted field is achieved through this direct tailoring of the exciting visible intensity. The results are in agreement with a simulation with no adjustable parameter.

Planar waveguides formed by Ag+-Na+ ion exchange in nonlinear optical glasses: diffusion and optical properties.

All-optical communication systems are the subject of intense research related to the integration of nonlinear optical materials. In sodiocalcic borophosphate glasses that contain niobium oxide and exhibit high nonlinear optical indices, planar waveguides have been formed by a Ag(+)-Na(+) ion-exchange technique. WKB analysis has been used to characterize the diffusion profiles of silver ions exchanged in glass substrate samples chemically by an electron microprobe technique and optically by an M-line technique. These methods permit the Ag(+) penetration depth and diffusion profile shape and index profiles to be determined. The results are analyzed and discussed in relation to Ca(2+) concentration and exchange conditions in glasses. The Ag(+) diffusion in these glasses can be almost entirely controlled for index-profile engineering.

Measurements of complex third-order optical susceptibility in a collinear pump-probe experiment.

We demonstrate simultaneous measurement of the real and the imaginary parts of third-order susceptibilities by use of a collinear pump-probe technique. This technique allows for good results and simple implementation. The signal analysis is based on the particular oscillatory signature versus the pump-probe delay allowed by the collinear configuration. Results are compared with interferometric measurements of a SF59 (Schott) glass sample.