Optical and structural characterization of femtosecond laser written micro-structures in germanate glass.

We report on direct femtosecond laser writing in zinc barium gallo-germanate glasses. A combination of spectroscopic techniques allows to progress in the understanding of the mechanisms taking place depending on the energy. In the first regime (type I, isotropic local index change) up to 0.

Hyper-Rayleigh Scattering as a New Chiroptical Method: Uncovering the Nonlinear Optical Activity of Aromatic Oligoamide Foldamers.

Molecular helices based on self-organized aromatic oligoamide foldamers have been designed and prepared in their two enantiomeric forms in order to probe their second-order nonlinear chiroptical properties in solution. The quinoline oligoamides were rationally functionalized by electron-donating and electron-withdrawing groups to afford a gradual increase of the electronic polarization of the helical architectures. Their hyper-Rayleigh scattering (HRS) responses in solution were accordingly assessed, using either linearly polarized or circularly polarized incident light.

Long-lived monolithic micro-optics for multispectral GRIN applications.

The potential for realizing robust, monolithic, near-surface refractive micro-optic elements with long-lived stability is demonstrated in visible and infrared transmitting glasses capable of use in dual band applications. Employing an enhanced understanding of glass chemistry and geometric control of mobile ion migration made possible with electrode patterning, flat, permanent, thermally-poled micro-optic structures have been produced and characterized. Sub-surface (t~5-10 µm) compositional and structural modification during the poling process results in formation of spatially-varying refractive index profiles, exhibiting induced Δn changes up to 5 × 10 which remain stable for >15 months.

Experimental and theoretical investigation of the first-order hyperpolarizability of octupolar merocyanine dyes.

Hyper-Rayleigh scattering experiments and quantum chemical calculations are combined to investigate the second-order nonlinear optical responses of a series of three-arm merocyanine derivatives. They exhibit an octupolar hyperpolarizability response with lower amplitude than crystal violet due to a lower extent of the photoinduced charge transfer and reduced bond length alternation. Strong effects on the second-order optical response measured close to the two-photon absorption level are clearly evidenced; for example, the effective measured polarization ratio deviates below the ideal octupolar value of 3/2 even at very low excitation power.

Preparation of a new electro-optic polymer cross-linkable via copper-free thermal Huisgen cyclo-addition and fabrication of optical waveguides by Reactive Ion Etching.

High-quality trails of ridge waveguides were successfully fabricated using a new cross-linkable polymer (PCC01) by UV photolithography followed by Reactive-Ion Etching (RIE) process. The cross-linking reaction of PCC01 is based on the copper-free Huisgen cyclo-addition between an azide and an acetylene group. The new cross-linkable polymer (PCC01) consists of a structural modification of the previously described materials (Scarpaci et al.

Local structure in ionic liquids investigated by hyper-Rayleigh scattering.

A series of ionic liquids involving imidazolium, pyrrolidinium, and alkyl ammonium cations with different anions (namely, [BF(4)], [PF(6)], [TFSI], [SCN], and [(CN)(2)N]) have been studied by hyper-Rayleigh scattering (HRS), which is a powerful technique to probe the local structure of liquids in a multipolar description. The interpretation of the HRS measurements in terms of an elementary structural (ES) entity has revealed a dominating octopolar nature of ES scatterers. By combining the HRS analysis with density functional theory calculations for different-sized ion pair clusters, we show that the octopolar nature to ES hyperpolarizability in ionic liquids (ILs) originates from a complex local structure due to the formation of 'transient' ion clusters within the time of observation of HRS (~10(-12) to 10(-14) s).

Two-way molecular switches with large nonlinear optical contrast.

Molecular switches: Highly efficient acido- and photoswitchable frequency doublers (see scheme) based on the indolinooxazolidine core are studied by means of hyper-Rayleigh experiments and quantum-chemical calculations.To optimize the nonlinear optical (NLO) contrast, a series of indolinooxazolidine derivatives with electron-withdrawing substituents in the para position on the indolinic residue have been synthesized. Their linear and nonlinear optical properties have been characterized by UV-visible absorption and hyper-Rayleigh scattering measurements, as well as by ab initio calculations.

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.

Acido-triggered nonlinear optical switches: benzazolo-oxazolidines.

This work is the continuation of our previous experimental and theoretical studies aiming at designing efficient nonlinear optical (NLO) switches derived from the benzazolo-oxazolidine core. Here, we report the synthesis and the characterization of the linear and nonlinear optical properties of benzothiazolo[2,3-b]oxazolidine acidochromes by means of hyper-Rayleigh scattering as well as quantum chemical calculations. It is shown that these new derivatives incorporating a benzothiazole subunit exhibit very high static first hyperpolarizability values in their acido-generated form.

Acido- and phototriggered NLO properties enhancement.

In this paper, acido- and phototriggered enhancement of the nonlinear optical (NLO) properties are achieved by combining the 10-(2-arylethenyl)indolino[2,1-b]oxazolidine unit with various styrylic residues. The synthetic pathway allows the preparation of phenyl, naphthyl, anthryl, and phenanthryl derivatives, which have been shown to display photochromic and acidochromic behavior at ambient temperature. The multiaddressable molecular switches are characterized by a large contrast of the NLO response along the reversible transformations.

Significant enhancement of the optical second harmonic generation in a poled azopolymer thin grating.

Nonlinear optical properties of an electrically poled surface relief grating inscribed on a thin film of azopolymer have been investigated. The linear and nonlinear optical far-field diffraction patterns of the grating are compared, and they show a clear angular separation of the fundamental (lambda = 1.064 mum) and second harmonic generated beams that are diffracted at different angles.

Acidoswitchable NLO-phores: benzimidazolo[2,3-b]oxazolidines.

This paper presents a series of acidoswitchable NLO-phores combining the 9-methylbenzimidazolo[2,3-b]oxazolidine core with various pi systems such as phenylethenyl, phenylethynyl, and naphthylethenyl. All the prepared derivatives are shown to display acidochromic behavior at ambient temperature. The remarkable contrast in the NLO response along the reversible transformations observed in HRS experiments is rationalized by high level theoretical calculations.

Large second-harmonic generation of thermally poled sodium borophosphate glasses.

Second harmonic generation (SHG) has been obtained in a rich in sodium niobium orophosphate glass by a thermal poling treatment. The thermally poled glass SHG signal has been studied through an original analysis of both transmitted and reflected polarized Maker-fringe patterns. Therefore, the second order nonlinear optical (NLO) efficiency was estimated from the simulation of the Maker-fringe patterns with a stepwise decreasing profile from the anode surface.