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International audience; Centimeter-sized single crystals of Ba2LaFeNb4O15 were grown from a high-temperature solution by using LiBO2 flux and a sealed platinum assembly. The obtained single crystals display the same physical properties as their ceramic counterparts. A frequency-dependent dielectric permittivity maximum was found (Tm = 100 K at 5 kHz), which indicates relaxor behavior. Magnetic susceptibility measurements revealed purely paramagnetic behavior between 10 and 350 K. X-ray diffraction measurements of Ba2LaFeNb4O15 single crystals revealed an incommensurate structure at room temperature with a bidimensional modulation characterized by vectors q1 = (α, α, 1/2) and q2 = (α, -α, 1/2) with α = 0.295(1). This crystal growth method offers a promising elaboration route to centimeter-sized crystals of niobate-based compounds, which may not be grown from the pure liquid phase, especially those with a tetragonal tungsten bronze (TTB) structure.

International audience; Tetragonal Tungsten Bronze Ferroelectrics (TTB) are currently revisited for the elaboration of new multifunctional materials. Recent studies on Ba2LnFeNb4O15 ceramics (Ln=Nd, Sm and Eu) demonstrated that these materials display both ferroelectric and ferromagnetic behaviors at room temperature due to the presence of barium hexaferrite as a secondary phase. In this paper, we report for the first time the growth of Ba2LnFeNb4O15 single crystals (Ln=La, Pr, Nd, Sm and Eu) from high temperature solution using LiBO2 flux. Inclusion free millimeter-sized single crystals were successfully grown. Structural and dielectric characterizations were performed and chemical analysis confirmed that the TTB matrix is reluctant to accommodate small rare earth as it was observed for ceramics. A paramagnetic behavior was observed for all compositions, which corroborates the composite nature of the TTB ceramic multiferroics at room temperature, while dielectric measurements on Ln=La and Pr crystals confirmed their relaxor behavior.

International audience; We have investigated the dielectric response of Ba2PrxNd1-xFeNb4O15 ceramics (x = 0, 0.2, 0.5, 0.6, 0.8, 1) in the frequency range from 20 Hz to 1 GHz. The obtained results confirmed the continuous transformation from the ferroelectric behavior of Ba2NdFeNb4O15 to the pure relaxor response of Ba2PrFeNb4O15 with increasing x. For intermediate x values, coexisting ferroelectric transition and relaxor dielectric signatures were observed, corresponding to two different phenomena in the framework of these materials. Increasing the amount of Pr decreases the ferroelectric phase transition temperatures in these ceramics; a large cooling??heating hysteresis exceeding 50K was also observed.

International audience; Relaxors are very interesting materials but most of the time they are restricted to perovskite materials and thus their flexibility is limited. We have previously shown that tetragonal tungsten bronze (TTB) niobate Ba2PrFeNb4O15 was a relaxor below 170 K and that Ba2NdFeNb4O15 displays a ferroelectric behavior with a TC = 323 K. On scanning the whole solid solution Ba2PrxNd1−xFeNb4O15 (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8 and 1), we demonstrate here a continuous crossover between these end member behaviors with a coexistence of ferroelectricity and relaxor in the intermediate range. This tunability is ascribed to the peculiar structure of the TTB networks which is more open than the classical perovskites. This allows for the coexistence of long range and short range orders and thus opens up the range of relaxor materials.

International audience; {Tb3}[Sc2−xLux](Al3)O12 crystals have been grown and investigated for the first time for magneto-optical applications. Tb3Al5O12 exhibits the best magneto-optical features; however, its incongruent melting nature has led to the industrial use of Tb3Ga5O12. Tb3Sc2Al3O12 had been proposed as an alternative to Tb3Al5O12, but unfortunately its growth also presents several drawbacks. The present investigation shows that by the isovalent substitution of Sc3+ by Lu3+ in the octahedral site of the garnet structure, it is possible to improve the growth characteristics while preserving the superior magneto-optical properties. We demonstrate that {Tb3}[Sc2−xLux](Al3)O12 crystals show a higher visible transparency and a larger Faraday rotation than Tb3Ga5O12 crystals. {Tb3}[Sc2−xLux](Al3)O12 is therefore a very promising material in particular for new magneto-optical applications in the visible-near IR wavelength region.

International audience; Recent studies of ceramics of formula Ba2LnFeNb4O15 (Ln=rare earth) with the “tetragonal tungsten bronze” (TTB) structure have correlated their room temperature multiferroics properties to the occurrence of barium ferrite parasitic phases. This work presents the elaboration of Ba2LaFeNb4O15 and Ba2EuFeNb4O15 composite samples with an excess of hematite in the TTB nominal composition. The influence of crystal-chemistry on the phase content and properties of Ba2LnFeNb4O15 TTB composites is discussed. A particular focus on the mechanisms related to the in-situ formation of barium ferrite is given. We show that we can control the spurious ferrite phase in TTB multiferroic composites and thus modulate their magnetic response.

Several Niobium oxides of formula Ba2LnFeNb4O15 (Ln = La, Pr, Nd, Sm, Eu, Gd) with the Tetragonal Tungsten Bronze (TTB) structure have been synthesised by conventional solid-state methods. The Neodymium, Samarium and Europium compounds are ferroelectric with Curie temperature ranging from 320 to 440K. The Praseodymium and Gadolinium compounds behave as relaxors below 170 and 300 K respectively. The Praseodymium, Neodymium, Samarium, Europium and Gadolinium compounds exhibit magnetic hysteresis loops at room temperature originating from traces of a barium ferrite secondary phase. The presence of both ferroelectric and magnetic hysteresis loops at room temperature allows considering these materials as composites multiferroic. Based on crystal-chemical analysis we propose some relationships between the introduction of Ln3+ ions in the TTB framework and the chemical, structural and physical properties of these materials., Revised version after identification of a spurious barium ferrite phase responsible for composite multiferroic properties at RT. Appearance of this parasitic phase is correlated to the crystal-chemistry of the Ba2LnFeNb4O15 TTBs. Submitted to Solid State Sciences. 27 pages, 7 figures, 3 tables

International audience; The present work reports the optimisation of the composition and elaboration process of Ba6−2xLn2xFe1+xNb9−xO30 (0.6 x