Abstract
Herein we report the synthesis of aluminum oxynitride (Al5O6N) doped with Eu2+ and Ce3+ and examine the effects of the dopant concentration and the nature of the rare-earth-containing precursor (europium and cerium oxides, Eu(acac)3, and Ce(acac)3) on its properties. At dopant concentrations above the solubility limit of rare-earth aluminates (EuAl12O19 and CeAl11O18) in aluminum oxynitride, we observed the formation of aluminum nitride and aluminum oxide (α-Al2O3) as individual phases. The concentration of the latter phase was higher when the rare-earth oxides were used. The emission intensity in the cathodoluminescence spectra of the samples was shown to have a maximum at Eu2+ and Ce3+ concentrations from 0.1 to 0.5 at %. Concentration quenching of luminescence was observed.
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Wilson, R.G., Schwartz, R.N., Abernathy, C.R., Pearton, S.J., Newman, N., Rubin, M., Fu, T., and Zavada, J.M., 1.54-μm photoluminescence from Erimplanted GaN and AlN, Appl. Phys. Lett., 1994, vol. 65, pp. 992–994.
Wu, X., Hömmerich, U., MacKenzie, J.D., Abernathy, C.R., Pearton, S.J., Wilson, R.G., Schwartz, R.N., and Zavada, J.M., Photoluminescence study of Erdoped AlN, J. Lumin., 1997, vols. 72–74, pp. 284–286.
Yu, F., Yang, J., Delsing, A.C.A., and Hintzen, B.H.T., Preparation, characterization and luminescence properties of porous Si3N4 ceramics with Eu2O3 as sintering additive, J. Lumin., 2010, vol. 130, pp. 2298–2304.
Warga, J., Li, R., Basu, S.N., and Negro, L.D., Erbium-doped silicon nanocrystals in silicon/silicon nitride superlattice structures: light emission and energy transfer, Phys. E (Amsterdam, Neth.), 2009, vol. 41, pp. 1040–1043.
Ueno, K., Gas pressure sintered silicon nitride containing praseodymium oxide as sintering aid, Int. J. High Technol. Ceram., 1987, vol. 3, no. 1, p. 90.
Schlieper, T., Milius, W., and Schnick, W.Z., Nitridosilicate. II[1]. Hochtemperatur-Synthesen und Kristallstrukturen von Sr2Si5N8 und Ba2Si5N8, Anorg. Allg. Chem., 1995, vol. 621, no. 8, pp. 1380–1384.
Xie, R.J., Hirosaki, N., Suehiro, T., Xu, F.F., and Mitomo, M., A simple, efficient synthetic route to Sr2Si5N8:Eu2+-based red phosphors for white lightemitting diodes, Chem. Mater., 2006, vol. 18, no. 23, pp. 5578–5583.
Piao, X.Q., Horikawa, T., Hanzawa, H., and Machida, K.I., Photoluminescence properties of Ca2Si5N8:Eu2+ nitride phosphor prepared by carbothermal reduction and nitridation method, Chem. Lett., 2006, vol. 35, pp. 334–335.
Aldabergenova, S.B., Frank, G., Strunk, H.P., Maqbool, M., Richardson, H.H., and Kordesch, M.E., Structure changes of AlN:Ho films with annealing and enhancement of the Ho3+ emission, J. Non-Cryst. Solids, 2006, vol. 352, pp. 1290–1293.
Brien, V., Miska, P., Rinnert, H., Genève, D., and Pigeat, P., Structural, chemical and optical characterizations of nanocrystallized AlN:Er thin films prepared by r.f. magnetron sputtering, Mater. Sci. Eng., B, 2008, vol. 146, pp. 200–203.
Dimitrova, V.I., Van Patten, P.G., Richardson, H., and Kordesch, M.E., Photo-, cathodo-, and electroluminescence studies of sputter deposited AlN:Er thin films, Appl. Surf. Sci., 2001, vols. 175–176, pp. 480–483.
Chen, C., Chen, W., Rainwater, B., Liu, L., Zhang, H., Liu, Y., Guo, X., Zhou, J., and Xie, E., M2Si5N8:Eu2+-based (M = Ca, Sr) red-emitting phosphors fabricated by nitrate reduction process, Opt. Mater., 2011, vol. 33, pp. 1585–1590.
Piao, X.Q., Horikawa, T., Hanzawa, H., and Machida, K.I., Characterization and luminescence properties of Sr2Si5N8:Eu2+ phosphor for white light-emitting-diode illumination, Appl. Phys. Lett., 2006, vol. 88, paper 161 908.
Li, Y.Q., van Steen, E.J., van Krevel, J.W.H., Botty, G., Delsing, A.C.A., DiSalvo, F.J., de With, G., and Hintzen, H.T., Luminescence properties of red-emitting M2Si5N8:Eu2+ (M = Ca, Sr, Ba) LED conversion phosphors, J. Alloys Compd., 2006, vol. 417, pp. 273–279.
Cheng, J.P., Agrawal, D., and Roy, R., Microwave synthesis of aluminum oxynitride (ALON), J. Mater. Sci. Lett., 1999, vol. 18, no. 24, pp. 1989–1990.
Kikkawa, S., Hatta, N., and Takedaz, T., Preparation of aluminum oxynitride by nitridation of a precursor derived from aluminum-glycine gel and the effects of the presence of europium, J. Am. Ceram. Soc., 2008, vol. 91, pp. 924–928.
Blasse, G., Energy transfer between inequivalent Eu2+ ions, J. Solid State Chem., 1986, vol. 62, no. 2, pp. 207–211.
Sakuma, K., Hirosaki, N., and Xie, R.-J., Red-shift of emission wavelength caused by reabsorption mechanism of europium activated Ca-α-SiAlON ceramic phosphors, J. Lumin., 2007, vol. 126, pp. 843–852.
Kargin, Yu.F., Akhmadullina, N.S., Lysenkov, A.S., Ashmarin, A.A., Ishchenko, A.V., Viktorov, L.V., Teslenko, O.S., Shul’gin, B.V., Spirina, A.V., Solomonov, V.I., and Solntsev, K.A., Synthesis and cathodoluminescence characteristics of europium-doped Ca-sialons, Inorg. Mater., 2012, vol. 48, no. 8, pp. 827–831.
Fei, Q.-N., Liu, Y.-H., Gu, T.-C., and Wang, D.-J., Color improvement of white-light through Mn-enhancing yellow-green emission of SrSi2O2N2:Eu phosphor for white light emitting diodes, J. Lumin., 2011, vol. 131, pp. 960–964.
Fu, R., Agathopoulos, S., Song, X., Zhao, X., He, H., and Yu, X., Influence of energy transfer from Ce3+ to Eu2+ on luminescence properties of Ca O2N2:Ce3+, Eu2+ phosphors, Opt. Mater., 2010, vol. 33, pp. 99–102.
Zheng, J. and Forslund, B., Carbothermal synthesis of aluminium oxynitride (ALON) powder: influence of starting materials and synthesis parameters, J. Eur. Ceram. Soc., 1995, vol. 15, pp. 1087–1110.
Willems, H.X., Hendrix, M.M.R.M., de With, G., and Metselaar, R., Thermodynamics of ALON II: phase relations, J. Eur. Ceram. Soc., 1992, vol. 10, pp. 339–346.
Kikkawa, S., Hatta, N., and Takedaz, T., Preparation of aluminum oxynitride by nitridation of a precursor derived from aluminum-glycine gel and the effects of the presence of europium, J. Am. Ceram. Soc., 2008, vol. 91, pp. 924–928.
Yin, L.J. and Xu, X., Synthesis and photoluminescence of Eu2+-Mg2+ co-doped γ-AlON phosphors, Mater. Lett., 2009, vol. 63, pp. 1511–1513.
Deng, L., Lei, J., Shi, Y., Lin, T., Ren, Y., and Xie, J., Photoluminescence of Tb3+/Ce3+ co-doped aluminum oxynitride powders, Mater. Lett., 2011, vol. 65, pp. 769–771.
Whan, R.E. and Crosby, G.B., Luminescence studies of rare earth complexes: benzoylacetonate and dibenzoylmethide chelates, J. Mol. Spectrosc., 1962, vol. 8, pp. 315–327.
Marchand, R., L’Haridon, P., and Laurent, Y., Structure cristalline de Eu2(II)SiO4β, J. Solid State Chem., 1978, vol. 24, no. 1, pp. 71–76.
De Graaf, D., Hintzen, H.T., Hampshire, S., and de With, G., Long wavelength Eu2+ emission in Eu-doped Y-Si-Al-O-N glasses, J. Eur. Ceram. Soc., 2003, vol. 23, pp. 1093–1097.
Caldwell, M.L., Martin, A.L., Dimitrova, V.I., Van Patten, P.G., and Kordesch, M.E., Emission properties of an amorphous AlN:Cr3+ thin-film phosphor, Appl. Phys. Lett., 2001, vol. 78, no. 9, pp. 1246–1248.
Lozykowski, H.J., Jadwisienczak, W.M., Bensaoula, A., and Monteiro, O., Luminescence and excitation mechanism of Pr, Eu, Tb and Tm ions implanted into AlN, Microelectron. J., 2005, vol. 36, pp. 453–455.
Lozykowski, H.J. and Jadwisienczak, W.M., Thermal quenching of luminescence and isovalent trap model for rare-earth-ion-doped AlN, Phys. Status Solidi B, 2007, vol. 244, no. 6, pp. 2109–2126.
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Original Russian Text © N.S. Akhmadullina, A.S. Lysenkov, A.A. Ashmarin, Yu.F. Kargin, A.V. Ishchenko, V.V. Yagodin, B.V. Shul’gin, 2015, published in Neorganicheskie Materialy, 2015, Vol. 51, No. 5, pp. 529–537.
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Akhmadullina, N.S., Lysenkov, A.S., Ashmarin, A.A. et al. Effect of dopant concentration on the phase composition and luminescence properties of Eu2+- and Ce3+-doped AlONs. Inorg Mater 51, 473–481 (2015). https://doi.org/10.1134/S0020168515050015
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DOI: https://doi.org/10.1134/S0020168515050015