Demonstration of Type A volume Bragg gratings inscribed with a femtosecond Gaussian-Bessel laser beam.

To our knowledge, we report on the first demonstration of Type A VBGs inscribed in silver-containing phosphate glasses by femtosecond laser writing. The gratings are inscribed plane-by-plane by scanning the voxel of a 1030 nm Gaussian-Bessel inscription beam. This results in a refractive-index modification zone, induced by the appearance of silver clusters, extending over a much larger depth than those obtained with standard Gaussian beams. As a result, a high diffraction efficiency of 95% at 632.8 nm is demonstrated for a 2-µm period transmission grating with a 150-µm effective thickness indicating a strong refractive-index modulation of 1.78 × 10-3. Meanwhile, a refractive-index modulation of 1.37 × 10-3 was observed at a wavelength of 1.55 µm. Thus, this work opens the avenue for highly effective femtosecond-written VBGs suitable for industrial applications.

Individual design of aberration-free intraocular lenses.

An analytical tool capable of easily calculating a new aspheric intraocular lens (IOL) (shape factor, aspherization) chosen to be designed as "aberration free" in terms of spherical aberration and/or coma is reported. In terms of retinal image quality, the theoretical performances given by the new proposed IOLs compare well with commercial IOLs.

Direct-laser-written integrated mid-IR directional couplers in a BGG glass.

The development of coherent sources and other optical components for the mid-infrared has been hampered by the lack of sturdy materials that can withstand high power radiation or exposition to harsh environment. BGG glasses are robust materials transmitting over the 2.5-5 µm region. We report here the direct femtosecond laser fabrication of efficient directional couplers integrated in a BGG glass chip. The photonic components are characterized from 2.1 to 4.2 µm and compared to similar structures inscribed in silica glass samples. At 2.85 µm, a 99% relative cross transmission is reported in BGG glass. The experimental measurements are in good agreement with the coupled mode theory for wavelengths up to 3.5 µm.

Five-Dimensional Optical Data Storage Based on Ellipse Orientation and Fluorescence Intensity in a Silver-Sensitized Commercial Glass.

Five-dimensional (5D) recording and decoding is demonstrated by using femtosecond direct laser writing in a silver-containing commercial glass. In particular, laser intensities and ellipse orientations generated by anamorphic focusing are employed to produce 5D data storage unit (3D for XYZ, 1D for the orientation of the elliptically-shaped data storage unit and 1D for its fluorescence intensity). In the recording process, two different images of a 4-bit bitmap format were simultaneously embedded in the medium by multiplexing the elliptical orientation of the laser focus and its intensity so as to access oriented elliptical patterns with independent fluorescence intensity. In the decoding process, two merged original images were successfully reconstructed by comparing each data storage unit with a fabricated calibration matrix of 16 × 16 levels for elliptic orientations and fluorescence intensities. We believe this technique can be applied to semi-permanent high-density data storage device.

Analytical solution of a personalized intraocular lens design for the correction of spherical aberration and coma of a pseudophakic eye.

This manuscript reports on a closed-form solution determining the personalized required shape of a new intraocular lens able to remove spherical aberration and coma of a pseudophakic eye. The proposed analytical method, within the framework of the Seidel theory of third-order optical aberrations, considers corneal conicities, fourth-order aspheric surface of the intraocular optics, pupil-shift effect and ocular kappa angle.

Femtosecond laser writing of near-surface waveguides for refractive-index sensing.

Femtosecond laser writing of optical waveguides and components in glasses has been a remarkably growing research field during the last two decades. However, such laser- inscribed optical components were mostly written within the volume of the glass due to the unavoidable ablation that arises when the focal spot is approaching the glass surface. This has generally limited the interaction of light with the surrounding medium thus preventing sensing functionality. In this paper, we present the inscription of surface and near-surface silver based waveguides in a silver containing glass with no need for additional processing as it is the case for standard type I waveguides. In addition, an ultra-sensitive refractive index sensor in a 1 cm glass chip is obtained based on near-surface waveguides interacting with liquid droplets acting as top-layer on the glass surface. Remarkably, the device exhibits a novel double-wing feature that sharpens the response and enhances its sensitivity. Our results highlight the advantages of silver based waveguides paving the way towards further surface based sensors in fibers.

Direct laser writing of a new type of waveguides in silver containing glasses.

Direct laser writing in glasses is a growing field of research in photonics since it provides a robust and efficient way to directly address 3D material structuring. Generally, direct laser writing in glasses induces physical modifications such as refractive index changes that have been classified under three different types (Type I, II & III). In a silver-containing zinc phosphate glass, direct laser writing additionally proceeds via the formation of silver clusters at the periphery of the interaction voxel. In this paper, we introduce a novel type of refractive index modification based on the creation of the photo-induced silver clusters allowing the inscription of a new type of optical waveguides. Various waveguides as well as a 50-50 beam splitter were written inside bulk glasses and characterized. The waveguiding properties observed in the bulk of such silver-containing glass samples were further transposed to ribbon shaped fibers made of the same material. Our results pave the way for the fabrication of 3D integrated circuits and fiber sensors with original fluorescent, nonlinear optical and plasmonic properties. The universality of these new findings should further extend in any silver-containing glasses that show similar laser-induced behavior in terms of silver cluster production.

Sub-diffraction-limited fluorescent patterns by tightly focusing polarized femtosecond vortex beams in a silver-containing glass.

We report that the shape and size of fluorescent patterns can be controlled by the focused laser intensity distribution, which depends on irradiation conditions as well as on the spin and orbital angular momenta being carried by light, inducing the formation of silver cluster patterns in a silver-containing zinc phosphate glass. In particular, we demonstrate that sub-diffraction-limited inner structures of fluorescent patterns can be generated by direct laser writing (DLW) with tightly focused femtosecond laser vortex beams as Laguerre-Gauss modes (LG0l) with linear and left-handed circular polarizations. We believe this technique, further combined with dual-color DLW, can be useful and powerful for developing structured light enabled nanostructures.

Dual-color control and inhibition of direct laser writing in silver-containing phosphate glasses.

We report on dual-color control of femtosecond direct laser writing (DLW) in a noncommercial silver-containing zinc phosphate glass, thanks to an additional illumination with a cw (continuous wave) UV laser, either after the femtosecond irradiation or simultaneously. By tuning the cw UV power, we demonstrate the tunable control and inhibition of the production efficiency of laser-induced fluorescent silver clusters, leading up to 100% inhibition for simultaneous co-illumination when the laser writing is performed close enough to the permanent structuring threshold. The role of the cw UV illumination is discussed in terms of inhibition of the silver cluster precursors or of dissolution of the laser-induced silver clusters. These results show the ability of laser writing inhibition in our photosensitive silver-containing phosphate glass, which is a necessary step to further develop super-resolution laser writing approaches, such as STED-like DLW, either of fluorescent silver clusters or of silver metallic nanoparticles with plasmonic properties.

Patterning linear and nonlinear optical properties of photosensitive glasses by femtosecond structured light.

We report on structured light-induced femtosecond direct laser writing (DLW) under tight focusing in non-commercial silver-containing zinc phosphate glass, which leads to original patterns of fluorescent silver clusters. These fluorescence topologies show unique features of frustrated diffusion of charged species, giving rise to distorted silver cluster spatial distributions. Fluorescence and second harmonic generation correlative microscopy demonstrate the realization of structured light-induced direct laser poling, resulting from a laser-induced permanent and stable electric field buried inside the modified glass. Thus, structured light-induced DLW remarkably enables both linear and nonlinear patterning. This work highlights the interest of optical phase engineering to obtain nontrivial beam profiles and subsequent photo-induced patterns that cannot be reached under Gaussian beam irradiation.

Laser action along and near the optic axis of a holmium-doped KY(WO4)2 crystal.

We demonstrate the first (to our knowledge) quasi-three-level conical refraction laser operating at 2 µm, with 1.6 W of output power at 2074 nm, using a holmium-doped KY(WO4)2 crystal. A maximum slope efficiency of 52% has been achieved, along the optic axis with respect to the absorbed pump power. Furthermore, lasing operation around the optic axis has been performed. In this case, a maximum output power of 3 W has been reached, with a slope efficiency better than 70%, which are the best performances ever reported on this material.

Enhancement of nanograting formation assisted by silver ions in a sodium gallophosphate glass.

We investigated the influence of silver ions during the direct femtosecond laser-induced formation of nanogratings (NGs) at the surface of a tailored sodium gallophosphate glass. We observed that the silver ions had a remarkable influence because the silver-containing glass showed (1) lower fluence thresholds for the formation of the NGs; (2) much smoother NG shapes; and (3) a bifunctional behavior because fluorescence from laser-induced silver clusters occurs prior to the formation of the NGs. We demonstrate for the first time, to our knowledge, the formation of NGs assisted by noble metal ions, such as ions playing a kind of catalytic-like role that enhances and improves the NG formation and its incubation process. Our innovative approach provides promising potential for further improvements in processes for NG formation.

Chemometrics applied to quantitative analysis of ternary mixtures by terahertz spectroscopy.

Chemometrics was applied to qualitative and quantitative analyses of terahertz spectra obtained in transmission mode. A series of mixtures of three pure analytes, namely, citric acid, D-(-)fructose, and α-lactose monohydrate under various concentrations, was prepared as pressed pellets with polyethylene as binder. Then, terahertz absorbance spectra were recorded by terahertz time domain spectroscopy and analyzed. First, principal component analysis allowed one to correctly locate the samples into a ternary diagram. Second, quantitative analysis was achieved by partial least-squares (PLS) regression and artificial neural networks (ANN). The concentrations were predicted with values of relative mean square error lower than 0.9% for the three constituents. As a conclusion, chemometrics was demonstrated to be very efficient for the analysis of the ternary mixtures prepared for this study.

Examination of femtosecond laser matter interaction in multipulse regime for surface nanopatterning of vitreous substrates.

The paper presents our results on laser micro- and nanostructuring of sodium aluminosilicate glass for the permanent storage purposes and photonics applications. Surface structuring is realized by fs laser irradiation followed by the subsequent etching in a potassium hydroxide (10M@80 °C) for 1 to 10 minutes. As the energy deposited is lower than the damage and/or ablation threshold, the chemical etching permits to produce small craters in the laser modified region. The laser parameters dependent interaction regimes are revealed by microscopic analysis (SEM and AFM). The influence of etching time on craters formation is investigated under different incident energies, number of pulses and polarization states.

Three-dimensional direct femtosecond laser writing of second-order nonlinearities in glass.

We demonstrate that direct femtosecond laser writing in silver-containing zinc and gallium phosphate glass enables generation of three-dimensional (3D) optical second-order nonlinear microstructures having an χ(2) value about 2.5 times that of quartz. The proposed physical model involves photo-reduction, photo-dissociation, and migration of silver species within the glass matrix. 3D laser-written second-order nonlinear structures could become a new class of nonlinear optical components.

In situ semi-quantitative analysis of polluted soils by laser-induced breakdown spectroscopy (LIBS).

Time-saving, low-cost analyses of soil contamination are required to ensure fast and efficient pollution removal and remedial operations. In this work, laser-induced breakdown spectroscopy (LIBS) has been successfully applied to in situ analyses of polluted soils, providing direct semi-quantitative information about the extent of pollution. A field campaign has been carried out in Brittany (France) on a site presenting high levels of heavy metal concentrations. Results on iron as a major component as well as on lead and copper as minor components are reported. Soil samples were dried and prepared as pressed pellets to minimize the effects of moisture and density on the results. LIBS analyses were performed with a Nd:YAG laser operating at 1064 nm, 60 mJ per 10 ns pulse, at a repetition rate of 10 Hz with a diameter of 500 µm on the sample surface. Good correlations were obtained between the LIBS signals and the values of concentrations deduced from inductively coupled plasma atomic emission spectroscopy (ICP-AES). This result proves that LIBS is an efficient method for optimizing sampling operations. Indeed, "LIBS maps" were established directly on-site, providing valuable assistance in optimizing the selection of the most relevant samples for future expensive and time-consuming laboratory analysis and avoiding useless analyses of very similar samples. Finally, it is emphasized that in situ LIBS is not described here as an alternative quantitative analytical method to the usual laboratory measurements but simply as an efficient time-saving tool to optimize sampling operations and to drastically reduce the number of soil samples to be analyzed, thus reducing costs. The detection limits of 200 ppm for lead and 80 ppm for copper reported here are compatible with the thresholds of toxicity; thus, this in situ LIBS campaign was fully validated for these two elements. Consequently, further experiments are planned to extend this study to other chemical elements and other matrices of soils.

Cross-correlation technique for dispersion characterization of chirped volume Bragg gratings.

We propose using cross-correlation frequency-resolved optical gating for dispersion characterization of optical elements with high dispersion, such as ultrashort pulse stretchers and compressors. The technique is based on spectrally resolved second-order cross correlation (sum frequency generation) of a stretched pulse with a reference short pulse. Dispersion of optical elements with a high pulse stretching ratio can be completely characterized using this method, even with moderate resolution of spectral measurements of the cross-correlation signal. The proposed technique is used to measure dispersion of a chirped Bragg grating recorded in photo-thermo-refractive glass. It was found that dispersion of these gratings is almost linear with wavelength and has approximately the same slope with opposite signs for two orientations of the grating with opposite faces of the grating used as the input face. Analysis of higher-order dispersion of the grating shows some variations of dispersion across the aperture of the grating, mostly in the amount of third-order dispersion contribution.

Ultrashort laser pulse diffraction by transmitting volume Bragg gratings in photo-thermo-refractive glass.

We report on the characteristics of ultrashort laser pulse diffraction by transmitting volume Bragg gratings recorded in photo-thermo-refractive glass. The angular and spectral selectivity properties of these phase volume gratings are shown to obey the predictions of a modified Kogelnik's coupled wave analysis that accounts for polychromatic beams. Spatio-temporal distortions such as angular dispersion and pulse front tilt that occur after diffraction by a single volume grating are studied and corrected by using a volume grating pair. The angular filtering properties of volume gratings offer potential as spatial filtering elements inside ultrafast laser cavities.

Beat the diffraction limit in 3D direct laser writing in photosensitive glass.

Three-dimensional (3D) femtosecond laser direct structuring in transparent materials is widely used for photonic applications. However, the structure size is limited by the optical diffraction. Here we report on a direct laser writing technique that produces subwavelength nanostructures independently of the experimental limiting factors. We demonstrate 3D nanostructures of arbitrary patterns with feature sizes down to 80 nm, less than one tenth of the laser processing wavelength. Its ease of implementation for novel nanostructuring, with its accompanying high precision will open new opportunities for the fabrication of nanostructures for plasmonic and photonic devices and for applications in metamaterials.