Structural Rearrangement of a-SiOx:H Films with Pulse Photon Annealing

V. Terekhov, E. Terukov, Yury K. Undalov, K. Barkov, I. Zanin, O. V. Serbin, I. N. Trapeznikova
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The results of investigations on the crystallization of silicon nanoclusters in a SiOx matrix have shownthat, even a very fast method of annealing using PPA leads to the formation of large silicon crystallites. This also causes the crystallization of at least a part of the oxide phase in the form of silicon hydroxide H6O7Si2. Moreover, in films with an initial content of pure silicon nanoclusters ≤ 50%, during annealing a part of the silicon is spent on the formation of oxide, and part of it is spent on the formation of silicon crystals. While in a film with an initial concentration of silicon nanoclusters ≥ 53%, on the contrary, upon annealing, there occurs a partial transition of silicon from the oxide phase to the growth ofSi crystals  \n  \n  \n  \nReference \n1. Undalov Y. K., Terukov E. I., Silicon nanoclustersncl-Si in a hydrogenated amorphous silicon suboxidematrix a-SiOx:H (0 < x < 2). Semiconductors. 2015;49(7):867- 878. DOI: https://doi.org/10.1134/S10637826150702222. Kim K. H., Johnson E. V., Kazanskii A. G.,Khenkin M. V., Roca P. Unravelling a simple methodfor the low temperature synthesis of siliconnanocrystals and monolithic nanocrystalline thinfilms. Scientific Reports. 2017;7(1) DOI: https://doi.org/10.1038/srep405533. Undalov Y. K., Terukov E. I., Trapeznikova I. N.Formation of ncl-Si in the amorphous matrix a-SiOx-:H located near the anode and on the cathode, usinga time-modulated DC plasma with the (SiH4–Ar–O2)gas phase (Co2 = 21.5 mol%). Semiconductors.2019;53(11): 1514–1523. DOI: https://doi.org/10.1134/S10637826191102284. Terekhov V. A., Terukov E. I., Undalov Y. K.,Parinova E. V., Spirin D. E., Seredin P. V., Minakov D. A.,Domashevskaya E. P. Composition and optical propertiesof amorphous a-SiOx:H films with silicon nanoclusters.Semiconductors. 2016;50(2): 212–216. DOI:https://doi.org/10.1134/S10637826160202515. Terekhov V. A., Turishchev S. Y., Kashkarov V. M.,Domashevskaya E. P., Mikhailov A. N., Tetel’baum D. I.Silicon nanocrystals in SiO2 matrix obtained by ionimplantation under cyclic dose accumulation. PhysicaE: Low-dimensional Systems and Nanostructures.2007;38(1-2): 16–20. DOI: https://doi.org/10.1016/j.physe.2006.12.0306. Terekhov V. A., Turishchev S. Y., Pankov K. N.,Zanin I. E., Domashevskaya E. P., Tetelbaum D. I.,Mikhailov A. N., Belov A. I., Nikolichev D. E., Zubkov S. Y.XANES, USXES and XPS investigations of electronenergy and atomic structure peculiarities of the siliconsuboxide thin film surface layers containing Si nanocrystals.Surface and Interface Analysis. 2010;42(6-7):891–896. DOI: https://doi.org/10.1002/sia.33387. Terekhov V. A., Turishchev S. Y., Pankov K. N.,Zanin I. E., Domashevskaya E. P., Tetelbaum, MikhailovA. N., Belov A. I., Nikolichev D. E. Synchrotron investigationsof electronic and atomic-structure peculiaritiesfor silicon-oxide films’ surface layers containingsilicon nanocrystals. Journal of Surface Investigation.X-ray, Synchrotron and Neutron Techniques. 2011;5(5):958–967. DOI: https://doi.org/10.1134/S102745101110020X8. Sato K., Izumi T., Iwase M., Show Y., Morisaki H.,Yaguchi T., Kamino T. Nucleation and growth of nanocrystallinesilicon studied by TEM, XPS and ESR.Applied Surface Science. 2003;216 (1-4): 376–381. DOI:https://doi.org/10.1016/S0169-4332(03)00445-89. Ledoux G., Gong J., Huisken F., Guillois O., ReynaudC. Photoluminescence of size-separated siliconnanocrystals: Confirmation of quantum confinement.Applied Physics Letters. 2002;80(25): 4834–4836. DOI:https://doi.org/10.1063/1.148530210. Patrone L., Nelson D., Safarov V. I., Sentis M.,Marine W., Giorgio S. Photoluminescence of siliconnanoclusters with reduced size dispersion producedby laser ablation. Journal of Applied Physics. 2000;87(8):3829–3837. DOI: https://doi.org/10.1063/1.37242111. Takeoka S., Fujii M., Hayashi S. Size-dependentphotoluminescence from surface-oxidized Si nanocrystalsin a weak confinement regime. Physical ReviewB. 2000;62(24): 16820–16825. DOI: https://doi.org/10.1103/PhysRevB.62.1682012. Ievlev V. M. Activation of solid-phase processesby radiation of gas-discharge lamps, Russian ChemicalReviews. 2013;82(9): 815–834. DOI: https://doi.org/10.1070/rc2013v082n09abeh00435713. Zimkina T. M., Fomichev V. A. Ultrasoft X-Rayspectroscopy. Leningrad: Leningrad State UniversityPubl.; 1971. 132 p.14. Wiech G., Feldhütter H. O., Šimůnek A. Electronicstructure of amorphous SiOx:H alloy filmsstudied by X-ray emission spectroscopy: Si K, Si L, andO K emission bands. Physical Review B. 1993;47(12):6981–6989. DOI: https://doi.org/10.1103/Phys-RevB.47.698115. Domashevskaya E. P., Peshkov Y. A., TerekhovV. A., Yurakov Y. A., Barkov K. A., Phase compositionof the buried silicon interlayers in the amorph o u s m u l t i l a y e r n a n o s t r u c t u r e s[(Co45Fe45Zr10)/a-Si:H]41 and [(Co45Fe45Zr10)35(Al2O3)65/a-Si:H]41. Surface and Interface Analysis.2018;50(12-13): 1265–1270. DOI: https://doi.org/10.1002/sia.651516. Terekhov V. A., Kashkarov V. M., ManukovskiiE. Yu., Schukarev A. V., Domashevskaya E. P.Determination of the phase composition of surfacelayers of porous silicon by ultrasoft X-ray spectroscopyand X-ray photoelectron spectroscopy techniques.Journal of Electron Spectroscopy and Related Phenomena.2001;114–116: 895–900. DOI: https://doi.org/10.1016/S0368-2048(00)00393-517. JCPDS-International Centre for DiffractionData ICDD PDF-2, (n.d.) card No 01-077-2110.18. 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Abstract

Amorphous SiOx films with silicon nanoclusters are a new interesting material from the standpoint of the physics, technology, and possible practical applications, since such films can exhibit photoluminescence due to size quantization. Moreover, the optical properties of these structures can be controlled by varying the size and the content of silicon nanoclusters in the SiOx film, as well as by transforming nanoclusters into nanocrystals by means of high-temperature annealing. However, during the annealing of nonstoichiometric silicon oxide, significant changes can occur in the phase composition and the structure of the films. The results of investigations on the crystallization of silicon nanoclusters in a SiOx matrix have shownthat, even a very fast method of annealing using PPA leads to the formation of large silicon crystallites. This also causes the crystallization of at least a part of the oxide phase in the form of silicon hydroxide H6O7Si2. Moreover, in films with an initial content of pure silicon nanoclusters ≤ 50%, during annealing a part of the silicon is spent on the formation of oxide, and part of it is spent on the formation of silicon crystals. While in a film with an initial concentration of silicon nanoclusters ≥ 53%, on the contrary, upon annealing, there occurs a partial transition of silicon from the oxide phase to the growth ofSi crystals        Reference 1. Undalov Y. K., Terukov E. I., Silicon nanoclustersncl-Si in a hydrogenated amorphous silicon suboxidematrix a-SiOx:H (0 < x < 2). Semiconductors. 2015;49(7):867- 878. DOI: https://doi.org/10.1134/S10637826150702222. Kim K. H., Johnson E. V., Kazanskii A. G.,Khenkin M. V., Roca P. Unravelling a simple methodfor the low temperature synthesis of siliconnanocrystals and monolithic nanocrystalline thinfilms. Scientific Reports. 2017;7(1) DOI: https://doi.org/10.1038/srep405533. Undalov Y. K., Terukov E. I., Trapeznikova I. N.Formation of ncl-Si in the amorphous matrix a-SiOx-:H located near the anode and on the cathode, usinga time-modulated DC plasma with the (SiH4–Ar–O2)gas phase (Co2 = 21.5 mol%). Semiconductors.2019;53(11): 1514–1523. DOI: https://doi.org/10.1134/S10637826191102284. Terekhov V. A., Terukov E. I., Undalov Y. K.,Parinova E. V., Spirin D. E., Seredin P. V., Minakov D. A.,Domashevskaya E. P. Composition and optical propertiesof amorphous a-SiOx:H films with silicon nanoclusters.Semiconductors. 2016;50(2): 212–216. DOI:https://doi.org/10.1134/S10637826160202515. Terekhov V. A., Turishchev S. Y., Kashkarov V. M.,Domashevskaya E. P., Mikhailov A. N., Tetel’baum D. I.Silicon nanocrystals in SiO2 matrix obtained by ionimplantation under cyclic dose accumulation. PhysicaE: Low-dimensional Systems and Nanostructures.2007;38(1-2): 16–20. DOI: https://doi.org/10.1016/j.physe.2006.12.0306. Terekhov V. A., Turishchev S. Y., Pankov K. N.,Zanin I. E., Domashevskaya E. P., Tetelbaum D. I.,Mikhailov A. N., Belov A. I., Nikolichev D. E., Zubkov S. Y.XANES, USXES and XPS investigations of electronenergy and atomic structure peculiarities of the siliconsuboxide thin film surface layers containing Si nanocrystals.Surface and Interface Analysis. 2010;42(6-7):891–896. DOI: https://doi.org/10.1002/sia.33387. Terekhov V. A., Turishchev S. Y., Pankov K. N.,Zanin I. E., Domashevskaya E. P., Tetelbaum, MikhailovA. N., Belov A. I., Nikolichev D. E. Synchrotron investigationsof electronic and atomic-structure peculiaritiesfor silicon-oxide films’ surface layers containingsilicon nanocrystals. Journal of Surface Investigation.X-ray, Synchrotron and Neutron Techniques. 2011;5(5):958–967. DOI: https://doi.org/10.1134/S102745101110020X8. Sato K., Izumi T., Iwase M., Show Y., Morisaki H.,Yaguchi T., Kamino T. Nucleation and growth of nanocrystallinesilicon studied by TEM, XPS and ESR.Applied Surface Science. 2003;216 (1-4): 376–381. DOI:https://doi.org/10.1016/S0169-4332(03)00445-89. Ledoux G., Gong J., Huisken F., Guillois O., ReynaudC. Photoluminescence of size-separated siliconnanocrystals: Confirmation of quantum confinement.Applied Physics Letters. 2002;80(25): 4834–4836. DOI:https://doi.org/10.1063/1.148530210. Patrone L., Nelson D., Safarov V. I., Sentis M.,Marine W., Giorgio S. Photoluminescence of siliconnanoclusters with reduced size dispersion producedby laser ablation. Journal of Applied Physics. 2000;87(8):3829–3837. DOI: https://doi.org/10.1063/1.37242111. Takeoka S., Fujii M., Hayashi S. Size-dependentphotoluminescence from surface-oxidized Si nanocrystalsin a weak confinement regime. Physical ReviewB. 2000;62(24): 16820–16825. DOI: https://doi.org/10.1103/PhysRevB.62.1682012. Ievlev V. M. Activation of solid-phase processesby radiation of gas-discharge lamps, Russian ChemicalReviews. 2013;82(9): 815–834. DOI: https://doi.org/10.1070/rc2013v082n09abeh00435713. Zimkina T. M., Fomichev V. A. Ultrasoft X-Rayspectroscopy. Leningrad: Leningrad State UniversityPubl.; 1971. 132 p.14. Wiech G., Feldhütter H. O., Šimůnek A. Electronicstructure of amorphous SiOx:H alloy filmsstudied by X-ray emission spectroscopy: Si K, Si L, andO K emission bands. Physical Review B. 1993;47(12):6981–6989. DOI: https://doi.org/10.1103/Phys-RevB.47.698115. Domashevskaya E. P., Peshkov Y. A., TerekhovV. A., Yurakov Y. A., Barkov K. A., Phase compositionof the buried silicon interlayers in the amorph o u s m u l t i l a y e r n a n o s t r u c t u r e s[(Co45Fe45Zr10)/a-Si:H]41 and [(Co45Fe45Zr10)35(Al2O3)65/a-Si:H]41. Surface and Interface Analysis.2018;50(12-13): 1265–1270. DOI: https://doi.org/10.1002/sia.651516. Terekhov V. A., Kashkarov V. M., ManukovskiiE. Yu., Schukarev A. V., Domashevskaya E. P.Determination of the phase composition of surfacelayers of porous silicon by ultrasoft X-ray spectroscopyand X-ray photoelectron spectroscopy techniques.Journal of Electron Spectroscopy and Related Phenomena.2001;114–116: 895–900. DOI: https://doi.org/10.1016/S0368-2048(00)00393-517. JCPDS-International Centre for DiffractionData ICDD PDF-2, (n.d.) card No 01-077-2110.18. JCPDS-International Centre for DiffractionData ICDD PDF-2, (n.d.) card No 00-050-0438.
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脉冲光子退火法研究a-SiOx:H薄膜的结构重排
用x射线发射光谱研究了非晶SiOx:H合金薄膜的电子结构:Si K、Si L和do K发射带。物理学报。1993;47(12):681 - 689。DOI: https://doi.org/10.1103/Phys-RevB.47.698115。多马舍夫斯卡娅E. P.,佩什科夫Y. A.,捷列霍夫。刘志强,刘志强,刘志强,等。硅晶间层的相组成研究[(Co45Fe45Zr10)/ A - si:H]41和[(Co45Fe45Zr10)35(Al2O3)65/ A - si:H]41。表面与界面分析,2018;50(12-13):1265-1270。DOI: https://doi.org/10.1002/sia.651516。捷列霍夫V. A.,卡什卡罗夫V. M.,马努科夫斯基。余。A. V., Domashevskaya E. p .用超软x射线光谱和x射线光电子能谱技术测定多孔硅表面层的相组成。电子光谱与相关现象。2001;114-116:895-900。DOI: https://doi.org/10.1016/s0368 - 2048(00) 00393 - 517。国际衍射数据中心ICDD PDF-2, (n.d)卡号01-077-2110.18。国际衍射数据中心ICDD PDF-2, (n.d)卡号00-050-0438。
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