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.

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.

Development and experimental demonstration of negative first-order quasi-phase matching in a periodically poled Rb-doped KTiOPO4 crystal.

We worked on a new scheme of quasi-phase matching (QPM) based on the negative first order of the spatial modulation of the sign of the second-order nonlinearity. Applying this scheme in the case of angular-QPM (AQPM) in a biaxial crystal reveals new directions of propagation for efficient parametric frequency conversion as well as "giant" spectral acceptances. The experimental validation is performed in a periodically poled rubidium-doped KTiOPO4 biaxial crystal. This new approach naturally extends to other periodically poled uniaxial crystals such as periodically poled LiNbO3.

Radiation-Induced Defects and Effects in Germanate and Tellurite Glasses.

This review focuses on the radiation-induced changes in germanate and tellurite glasses. These glasses have been of great interest due to their remarkable potential for photonics, in terms of extended transmission window in the mid-infrared, ability of rare-earth loading suitable with a laser, and amplification in the near- and mid-infrared or high nonlinear optical properties. Here, we summarize information about possible radiation-induced defects, mechanisms of their formation, and the influence of the glass composition on this process. Special attention is paid to laser-induced structural modification of these glasses, including possible mechanisms of the laser-glass interaction, laser-induced crystallization, and waveguide writing. It is shown that these methods can be used for photostructuring of the glass and have great potential for practical applications.

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.

Study of middle infrared difference frequency generation using a femtosecond laser source in LGT.

We demonstrate phase-matched difference frequency generation in the emerging nonlinear crystal La3Ga5.5Ta0.5O14. Tunable wavelengths between 1.4 and 4.7 µm are generated by using femtosecond sources. We also report on the measurements of the optical damage threshold in the femtosecond regime and on the nonlinear refractive index n2.

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.

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.

Gold nanorods with phase-changing polymer corona for remotely near-infrared-triggered drug release.

Herein, we report a new drug-delivery system (DDS) that is comprised of a near-infrared (NIR)-light-sensitive gold-nanorod (GNR) core and a phase-changing poly(ε-caprolactone)-b-poly(ethylene glycol) polymer corona (GNR@PCL-b-PEG). The underlying mechanism of the drug-loading and triggered-release behaviors involves the entrapment of drug payloads among the PCL crystallites and a heat-induced phase change, respectively. A low premature release of the pre-loaded doxorubicin was observed in PBS buffer (pH 7.4) at 37 °C (<10% of the entire payload after 48 h). However, release could be activated within 30 min by conventional heating at 50 °C, above the Tm of the crystalline PCL domain (43.5 °C), with about 60% release over the subsequent 42 h at 37 °C. The NIR-induced heating of an aqueous suspension of GNR@PCL-b-PEG under NIR irradiation (802 nm) was investigated in terms of the irradiation period, power, and concentration-dependent heating behavior, as well as the NIR-induced shape-transformation of the GNR cores. Remotely NIR-triggered release was also explored upon NIR irradiation for 30 min and about 70% release was achieved in the following 42 h at 37 °C, with a mild warming (<4 °C) of the surroundings. The cytotoxicity of GNR@PCL-b-PEG against the mouse fibroblastic-like L929 cell-line was assessed by MTS assay and good compatibility was confirmed with a cell viability of over 90% after incubation for 72 h. The cellular uptake of GNR@PCL-b-PEG by melanoma MEL-5 cells was also confirmed, with an averaged uptake of 1250(±110) particles cell(-1) after incubation for 12 h (50 µg mL(-1)). This GNR@PCL-b-PEG DDS is aimed at addressing the different requirements for therapeutic treatments and is envisaged to provide new insights into DDS targeting for remotely triggered release by NIR activation.

Laser-induced plasma cloud interaction and ice multiplication under cirrus cloud conditions.

Potential impacts of lightning-induced plasma on cloud ice formation and precipitation have been a subject of debate for decades. Here, we report on the interaction of laser-generated plasma channels with water and ice clouds observed in a large cloud simulation chamber. Under the conditions of a typical storm cloud, in which ice and supercooled water coexist, no direct influence of the plasma channels on ice formation or precipitation processes could be detected. Under conditions typical for thin cirrus ice clouds, however, the plasma channels induced a surprisingly strong effect of ice multiplication. Within a few minutes, the laser action led to a strong enhancement of the total ice particle number density in the chamber by up to a factor of 100, even though only a 10(-9) fraction of the chamber volume was exposed to the plasma channels. The newly formed ice particles quickly reduced the water vapor pressure to ice saturation, thereby increasing the cloud optical thickness by up to three orders of magnitude. A model relying on the complete vaporization of ice particles in the laser filament and the condensation of the resulting water vapor on plasma ions reproduces our experimental findings. This surprising effect might open new perspectives for remote sensing of water vapor and ice in the upper troposphere.

Rotation of the absorption frame as a function of the electronic transition in the Nd3+:YCa4O(BO3)3 monoclinic crystal.

We report the first measurements of the angular distribution of absorption under polarized light corresponding to seven electronic transitions of Nd(3+) ions in the monoclinic crystal Nd:YCOB, revealing a rotation of the symmetry axes of the different patterns.

Singular topology of optical absorption in biaxial crystals.

We show for the first time that biaxial crystals exhibit continua of directions of propagation where the absorption coefficient is the same for the two associated polarization modes. This statement is supported by both calculations and experimental data obtained in Nd:YCOB.

Angular quasi-phase-matching experiments and determination of accurate Sellmeier equations for 5%MgO:PPLN.

We validated the theory of angular quasi-phase-matching (AQPM) by performing measurements of second-harmonic generation and difference-frequency generation. A nonlinear least-squares fitting of these experimental data led to refine the Sellmeier equations of 5%MgO:PPLN that are now valid over the complete transparency range of the crystal. We also showed that AQPM exhibits complementary spectral ranges and acceptances compared with birefringence phase matching.

Absorption and fluorescence anisotropies of monoclinic crystals: the case of Nd:YCOB.

We report for the first time measurements and modelization of the angular distributions of absorption and fluorescence in a monoclinic crystal. Studies on Nd:YCOB revealed specific topologies with ombilics. These new data upgrade the knowledge on low symmetry crystal optics.