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Ba2AlSi5N9—A New Host Lattice for Eu2+-Doped Luminescent Materials Comprising a Nitridoalumosilicate Framework with Corner- and Edge-Sharing Tetrahedra

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    Ba2AlSi5N9—A New Host Lattice for Eu2+-Doped Luminescent Materials Comprising a Nitridoalumosilicate Framework with Corner- and Edge-Sharing Tetrahedra
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    Department Chemie und Biochemie, Ludwig-Maximilians-Universität München, Butenandtstrasse 5-13 (D), D-81377 München, Germany, and Philips Technologie GmbH, Forschungslaboratorien, Solid State Lighting, Weisshausstrasse 2, D-52066 Aachen, Germany
    * To whom correspondence should be addressed. Fax: ( +49)89-2180-77440. E-mail: [email protected]
    †Ludwig-Maximilians-Universität München.
    ‡Philips Technologie GmbH.
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    Chemistry of Materials

    Cite this: Chem. Mater. 2009, 21, 7, 1288–1295
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    https://doi.org/10.1021/cm803233d
    Published March 10, 2009
    Copyright © 2009 American Chemical Society
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    Abstract

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    Ba2AlSi5N9 was synthesized starting from Si3N4, AlN, and Ba in a radio-frequency furnace at temperatures of about 1725 °C. The new nitridoalumosilicate crystallizes in the triclinic space group P1 (no. 1), a = 9.860(1) Å, b = 10.320(1) Å, c = 10.346(1) Å, α = 90.37(2)°, β = 118.43(2)°; γ = 103.69(2)°, Z = 4, R1 = 0.0314. All synthesized crystals were characteristically twinned by reticular pseudomerohedry with twin law (1 0 0, −0.5 −1 0, −1 0 −1). The crystal structure of Ba2AlSi5N9 was determined from single-crystal X-ray diffraction data of a twinned crystal and confirmed by Rietveld refinement both on X-ray and on neutron powder diffraction data. Statistical distribution Si/Al is corroborated by lattice energy calculations (MAPLE). 29Si and 27Al solid-state NMR are in accordance with the crystallographic results. Ba2AlSi5N9 represents a new type of network structure made up of TN4 tetrahedra (T = Si, Al). Highly condensed layers of dreier rings with nitrogen connecting three neighboring tetrahedral centers occur which are further crosslinked by dreier rings and vierer rings. The dreier rings consist of corner-sharing tetrahedra, whereas some of the vierer rings exhibit two pairs of edge-sharing tetrahedra. In the resulting voids of the network there are eight different Ba2+ sites with coordination numbers between 6 and 10. Thermogravimetric investigations confirmed a thermal stability of Ba2AlSi5N9 up to about 1515 °C (He atmosphere). Luminescence measurements on Ba2AlSi5N9:Eu2+ (2 mol % Eu2+) with an excitation wavelength of 450 nm revealed a broadband emission peaking at 584 nm (FWHM = 100 nm) originating from dipole-allowed 4f6(7F)5d1 → 4f7(8S7/2) transitions.

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    The atomic coordinates, (equivalent) isotropic and anisotropic displacement parameter, and site occupancy factors of Ba2AlSi5N9 as well as selected bond length and angles. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: Chem. Mater. 2009, 21, 7, 1288–1295
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