The target of taking advantage of the near-infrared light-emission properties of nickel ions in crystals for the design of novel broadband optical amplifiers requires the identification of suitable nanostructured glasses able to embed Ni-doped nanocrystals and to preserve the workability of a glass. Here we show that Ni doping of Li(2)O-Na(2)O-Ga(2)O(3)-GeO(2)-SiO(2) glass (with composition 7.5:2.5:20:35:35 and melting temperature 1480 °C, sensibly lower than in Ge-free silicates) enables the selective embedding of nickel ions in thermally grown nanocrystals of spinel-like gallium oxide. The analysis of transmission electron microscopy and x-ray diffraction data as a function of Ni-content (from 0.01 to 1 mol%) indicates that Ni ions promote the nanophase crystallization without affecting nanoparticle size (~6 nm) and concentration (~4 × 10(18) cm(-3)). Importantly, as shown by optical absorption spectra, all nickel ions enter into the nanophase, with a number of ions per nanocrystal that depends on the nanocrystal concentration and ranges from 1 to 10(2). Photoluminescence data indicate that fast non-radiative decay processes become relevant only at mean ion-ion distances shorter than 1.4 nm, which enables the incorporation of a few Ni ions per nanoparticle without too large a worsening of the light-emission efficiency. Indeed, at 0.1 mol% nickel, the room temperature quantum yield is 9%, with an effective bandwidth of 320 nm.
Nanoparticles in amorphous oxides are a powerful tool for embedding a wide range of functions in optical glasses, which are still the best solutions in several applications in the ever growing field of photonics. However, the control of the nanoparticle size inside the host material is often a challenging task, even more challenging when detrimental effects on light transmittance have to be avoided. Here we show how the process of phase separation and subsequent nanocrystallization of a Ga-oxide phase can be controlled in germanosilicates - prototypal systems in optical telecommunications - starting from a Ga-modified glass composition designed to favour uniform liquid-liquid phase separation in the melt. Small angle neutron scattering data demonstrate that nanosized structuring occurs in the amorphous as-quenched glass and gives rise to initially smaller nanoparticles, by heating, as in a secondary phase separation. By further heating, the nanophase evolves with an increase of nanoparticle gyration radius, from a few nm to a saturation value of about 10 nm, through an initial growing process followed by an Ostwald ripening mechanism. Nanoparticles finally crystallize, as indicated by transmission electron microscopy and X-ray diffraction, as γ-Ga(2)O(3)- a metastable gallium oxide polymorph. Infrared reflectance and photoluminescence, together with the optical absorption of Ni ions used as a probe, give an indication of the underlying interrelated processes of the structural change in the glass and in the segregated phase. As a result, our data give for the first time a rationale for designing Ga-modified germanosilicates at the nanoscale, with the perspective of a detailed nanostructuring control.
We report the one-step precipitation of CdS quantum dots in the volume of CdS-doped silicate glass under the focused femtosecond laser beam without additional heat treatment of glass. Femtosecond direct laser writing leads to the annular distribution of the precipitated CdS quantum dots in laser-written domain optical properties of which could be tuned by laser beam parameters. Increasing the laser pulse number to 10 significantly enhances luminescence intensity in the domains, while further increasing up to 10 pulses leads to luminescence quenching. A possible scenario for the formation and distribution of quantum dots is proposed.
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