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- ItemGiant faraday rotation through ultra-small Fe0n clusters in superparamagnetic FeO-SiO2 vitreous films(Hoboken : Wiley, 2017) Nakatsuka, Yuko; Pollok, Kilian; Wieduwilt, Torsten; Langenhorst, Falko; Schmidt, Markus A.; Fujita, Koji; Murai, Shunsuke; Tanaka, Katsuhisa; Wondraczek, LotharMagnetooptical (MO) glasses and, in particular, Faraday rotators are becoming key components in lasers and optical information processing, light switching, coding, filtering, and sensing. The common design of such Faraday rotator materials follows a simple path: high Faraday rotation is achieved by maximizing the concentration of paramagnetic ion species in a given matrix material. However, this approach has reached its limits in terms of MO performance; hence, glass‐based materials can presently not be used efficiently in thin film MO applications. Here, a novel strategy which overcomes this limitation is demonstrated. Using vitreous films of xFeO·(100 − x)SiO2, unusually large Faraday rotation has been obtained, beating the performance of any other glassy material by up to two orders of magnitude. It is shown that this is due to the incorporation of small, ferromagnetic clusters of atomic iron which are generated in line during laser deposition and rapid condensation of the thin film, generating superparamagnetism. The size of these clusters underbids the present record of metallic Fe incorporation and experimental verification in glass matrices.
- ItemPlasma-based VAD process for multiply doped glass powders and high-performance fiber preforms with outstanding homogeneity(Hoboken, NJ : Wiley Interscience, 2020) Trautvetter, Tom; Schäfer, Jan; Benzine, Omar; Methling, Ralf; Baierl, Hardy; Reichel, Volker; Dellith, Jan; Köpp, Daniel; Hempel, Frank; Stankov, Marjan; Baeva, Margarita; Foest, Rüdiger; Wondraczek, Lothar; Wondraczek, Katrin; Bartelt, HartmutAn innovative approach using the vapor axial deposition (VAD), for the preparation of silica-based high-power fiber laser preforms, is described in this study. The VAD uses a plasma deposition system operating at atmospheric pressure, fed by a single, chemically adapted solution containing precursors of laser-active dopants (e.g., Yb2O3), glass-modifier species (e.g., Al2O3), and the silica matrix. The approach enables simultaneous doping with multiple optically active species and overcomes some of the current technological limitations encountered with well-established fiber preform technologies in terms of dopant distribution, doping levels, and achievable active core diameter. The deposition of co-doped silica with outstanding homogeneity is proven by Raman spectroscopy and electron probe microanalysis. Yb2O3 concentrations are realized up to 0.3 mol% in SiO2, with simultaneous doping of 3 mol% of Al2O3.
- ItemControlling Growth of Poly (Triethylene Glycol Acrylate-Co-Spiropyran Acrylate) Copolymer Liquid Films on a Hydrophilic Surface by Light and Temperature(Basel : MDPI, 2021) Ben-Miled, Aziz; Nabiyan, Afshin; Wondraczek, Katrin; Schacher, Felix H.; Wondraczek, LotharA quartz crystal microbalance with dissipation monitoring (QCM-D) was employed for in situ investigations of the effect of temperature and light on the conformational changes of a poly (triethylene glycol acrylate-co-spiropyran acrylate) (P (TEGA-co-SPA)) copolymer containing 12–14% of spiropyran at the silica–water interface. By monitoring shifts in resonance frequency and in acoustic dissipation as a function of temperature and illumination conditions, we investigated the evolution of viscoelastic properties of the P (TEGA-co-SPA)-rich wetting layer growing on the sensor, from which we deduced the characteristic coil-to-globule transition temperature, corresponding to the lower critical solution temperature (LCST) of the PTEGA part. We show that the coil-to-globule transition of the adsorbed copolymer being exposed to visible or UV light shifts to lower LCST as compared to the bulk solution: the transition temperature determined acoustically on the surface is 4 to 8 K lower than the cloud point temperature reported by UV/VIS spectroscopy in aqueous solution. We attribute our findings to non-equilibrium effects caused by confinement of the copolymer chains on the surface. Thermal stimuli and light can be used to manipulate the film formation process and the film’s conformational state, which affects its subsequent response behavior.
- ItemFluoride-Sulfophosphate/Silica Hybrid Fiber as a Platform for Optically Active Materials(Lausanne : Frontiers Media, 2019) Wang, Wei-Chao; Yang, Xu; Wieduwilt, Torsten; Schmidt, Markus A.; Zhang, Qin-Yuan; Wondraczek, LotharPressure-assisted melt filling (PAMF) of pre-fabricated micro-capillaries has been proven an effective way of fabricating hybrid optical fiber (HOF) from unusual combinations of materials. Here, we extend the applicability of PAMF to multi-anionic fluoride-sulfophosphate (FPS) glasses. FPS glasses provide extended transmission windows and high solubility for various transition metal (TM) and rare earth (RE) ion species. Using PAMF for fabricating FPS/silica HOFs can therefore act as a platform for a broad variety of optically active fiber devices. For the present demonstration purposes, we selected Cr3+- and Mn2+-doped FPS. For both glasses, we demonstrate how the spectral characteristics of the bulk material persist also in the HOF. Using a double-core fiber structure in which waveguiding is conducted in a primary GeO2-SiO2 core, mode coupling to the secondary FPS-filled core allows one to exploit the optical activity of the doped FPS glass even when the intrinsic optical loss is high.Pressure-assisted melt filling (PAMF) of pre-fabricated micro-capillaries has been proven an effective way of fabricating hybrid optical fiber (HOF) from unusual combinations of materials. Here, we extend the applicability of PAMF to multi-anionic fluoride-sulfophosphate (FPS) glasses. FPS glasses provide extended transmission windows and high solubility for various transition metal (TM) and rare earth (RE) ion species. Using PAMF for fabricating FPS/silica HOFs can therefore act as a platform for a broad variety of optically active fiber devices. For the present demonstration purposes, we selected Cr3+- and Mn2+-doped FPS. For both glasses, we demonstrate how the spectral characteristics of the bulk material persist also in the HOF. Using a double-core fiber structure in which waveguiding is conducted in a primary GeO2-SiO2 core, mode coupling to the secondary FPS-filled core allows one to exploit the optical activity of the doped FPS glass even when the intrinsic optical loss is high.
- ItemBoson peak, heterogeneity and intermediate-range order in binary SiO2-Al2O3 glasses(Berlin : Nature Publishing, 2018) Fatobene Ando, Mariana; Benzine, Omar; Pan, Zhiwen; Garden, Jean-Luc; Wondraczek, Katrin; Grimm, Stephan; Schuster, Kay; Wondraczek, LotharIn binary aluminosilicate liquids and glasses, heterogeneity on intermediate length scale is a crucial factor for optical fiber performance, determining the lower limit of optical attenuation and Rayleigh scattering, but also clustering and precipitation of optically active dopants, for example, in the fabrication of high-power laser gain media. Here, we consider the low-frequency vibrational modes of such materials for assessing structural heterogeneity on molecular scale. We determine the vibrational density of states VDoS g(ω) using low-temperature heat capacity data. From correlation with low-frequency Raman spectroscopy, we obtain the Raman coupling coefficient. Both experiments allow for the extraction of the average dynamic correlation length as a function of alumina content. We find that this value decreases from about 3.9 nm to 3.3 nm when mildly increasing the alumina content from zero (vitreous silica) to 7 mol%. At the same time, the average inter-particle distance increases slightly due to the presence of oxygen tricluster species. In accordance with Loewensteinian dynamics, this proves that mild alumina doping increases structural homogeneity on molecular scale.
- ItemStructural relaxation phenomena in silicate glasses modified by irradiation with femtosecond laser pulses(London : Nature Publishing Group, 2017) Seuthe, Thomas; Mermillod-Blondin, Alexandre; Grehn, Moritz; Bonse, Jörn; Wondraczek, Lothar; Eberstein, MarkusStructural relaxation phenomena in binary and multicomponent lithium silicate glasses were studied upon irradiation with femtosecond (fs) laser pulses (800 nm central wavelength, 130 fs pulse duration) and subsequent thermal annealing experiments. Depending on the annealing temperature, micro-Raman spectroscopy analyses evidenced different relaxation behaviours, associated to bridging and non-bridging oxygen structures present in the glass network. The results indicate that the mobility of lithium ions is an important factor during the glass modification with fs-laser pulses. Quantitative phase contrast imaging (spatial light interference microscopy) revealed that these fs-laser induced structural modifications are closely related to local changes in the refractive index of the material. The results establish a promising strategy for tailoring fs-laser sensitivity of glasses through structural mobility.
- ItemBiomimetic light dilution using side-emitting optical fiber for enhancing the productivity of microalgae reactors(Berlin : Nature Publishing, 2019) Wondraczek, Lothar; Gründler, Alexander; Reupert, Aaron; Wondraczek, Katrin; Schmidt, Markus A.; Pohnert, Georg; Nolte, StephanPhotoautotrophic microbes present vast opportunities for sustainable lipid production, CO2 storage and green chemistry, for example, using microalgae beds to generate biofuels. A major challenge of microalgae cultivation and other photochemical reactors is the efficiency of light delivery. In order to break even on large scale, dedicated photon management will be required across all levels of reactor hierarchy – from the harvesting of light and its efficient injection and distribution inside of the reactor to the design of optical antenna and pathways of energy transfer on molecular scale. Here, we discuss a biomimetic approach for light dilution which enables homogeneous illumination of large reactor volumes with high optical density. We show that the immersion of side-emitting optical fiber within the reactor can enhance the fraction of illuminated volume by more than two orders of magnitude already at cell densities as low as ~5 104ml−1. Using the green algae Haematococcus pluvialis as a model system, we demonstrate an increase in the rate of reproduction by up to 93%. Beyond micoralgae, the versatile properties of side-emitting fiber enable the injection and dilution of light with tailored spectral and temporal characteristics into virtually any reactor containment.
- ItemFaraday rotation and photoluminescence in heavily Tb(3+)-doped GeO2-B2O3-Al2O3-Ga2O3 glasses for fiber-integrated magneto-optics([London] : Macmillan Publishers Limited, part of Springer Nature, 2015) Gao, Guojun; Winterstein-Beckmann, Anja; Surzhenko, Oleksii; Dubs, Carsten; Dellith, Jan; Schmidt, Markus A.; Wondraczek, LotharWe report on the magneto-optical (MO) properties of heavily Tb3+-doped GeO2-B2O3-Al2O3-Ga2O3 glasses towards fiber-integrated paramagnetic MO devices. For a Tb3+ ion concentration of up to 9.7 × 1021 cm−3, the reported glass exhibits an absolute negative Faraday rotation of ~120 rad/T/m at 632.8 nm. The optimum spectral ratio between Verdet constant and light transmittance over the spectral window of 400–1500 nm is found for a Tb3+ concentration of ~6.5 × 1021 cm−3. For this glass, the crystallization stability, expressed as the difference between glass transition temperature and onset temperature of melt crystallization exceeds 100 K, which is a prerequisite for fiber drawing. In addition, a high activation energy of crystallization is achieved at this composition. Optical absorption occurs in the NUV and blue spectral region, accompanied by Tb3+ photoluminescence. In the heavily doped materials, a UV/blue-to-green photo-conversion gain of ~43% is achieved. The lifetime of photoluminescence is ~2.2 ms at a stimulated emission cross-section σem of ~1.1 × 10−21 cm2 for ~ 5.0 × 1021 cm−3 Tb3+. This results in an optical gain parameter σem*τ of ~2.5 × 10−24 cm2s, what could be of interest for implementation of a Tb3+ fiber laser.