The Density–Structure Correlations in Al2O3Glasses: Insights from Molecular Dynamics Simulation
Main Article Content
Abstract
The relationship between structure and density in Al2O3 glass has been studied by mean of molecular dynamic simulation. Simulation results reveal that the structure of Al2O3 is formed by AlOx structural unit. Under densification, there is the transformation from tetrahedral to octahedral structure. The AlOx structural units tend to form the cluster of AlOx units. Alumina exhibits polymorphism and heterogeneous structure due to the presence of AlOx clusters and two-domain types (D4–D5 or D5–D6) in the intermediate density range. Moreover, a continuous random network of basic structural units linking to each other via with corner-sharing, edge-sharing, face-sharing bond. At low density region, the basic structural units are mainly linked via bridge oxygen and the connectivity between AlOx is mainly corner sharing bonds. The numbers of corner-sharing and edge-sharing bonds vary in opposite directions. The basic structural units are barely bonded to each other via face-sharing bond. In the model, there is the existence of the free volume region. The distribution of free volumes depends on density. It has the Gaussian form and the position of the peak tends to shift to the left under compression. As densnit increases, the void radius decreases rapidly.
Keywords:
Molecular dynamic, structural transformation, structural heterogeneity, polymorphism, density.
References
[1] M. I. Ojovan, Viscosity and Glass Transition in Amorphous Oxides, Advances in Condensed Matter Physics,
Vol. 2008, 2008, pp. 817829, https://doi.org/10.1155/2008/817829.
[2] Y. Zhao, X. Bian, X. Hou, Viscosity and Fragility of the Supercooled and Superheated Liquids of the Ni₆₀Zr₃₀Al₁₀ Metallic Glass-forming Alloy, Physica A: Statistical Mechanics and its Applications, Vol. 367(C), 2006,
pp. 42-54, https://doi.org/10.1016/j.physa.2005.11.020.
[3] K. S. Shamala, L. C. S. Murthy, M. C. Radhakrishna, K. N. Rao, Characterization of Al₂O₃ thin Films Prepared by Spray Pyrolysis Method for Humidity Sensor, Sensors and Actuators A: Physical, Vol. 135, No. 2, 2007,
pp. 552-557, https://doi.org/10.1016/j.sna.2006.10.004.
[4] J. H. Park, T. Suzuki, M. Kurosawa, M. Miyao, T. Sadoh, Nucleation-Controlled Gold-Induced-Crystallization for Selective Formation of Ge(100) and (111) on Insulator at Low-Temperature (~250 °C), Applied Physics Letters, Vol. 103, No. 8, 2013, pp. 082102, https://doi.org/10.1063/1.4819015.
[5] Y. N. Novikov, V. A. Gritsenko, K. A. Nasyrov, Charge Transport Mechanism in Amorphous Alumina, Applied Physics Letters, Vol. 94, No. 22, 2009, pp. 222904, https://doi.org/10.1063/1.3151861.
[6] I. Jackson, Melting of the Silica Isotopes SiO₂, BeF₂ and GeO₂ at Elevated Pressures, Physics of the Earth and Planetary Interiors, Vol. 13, No. 3, 1976, pp. 218–231, https://doi.org/10.1016/0031-9201(76)90096-0.
[7] P. S. Salmon, A. Zeidler, Networks under Pressure: the Development of in Situ High-Pressure Neutron Diffraction for Glassy and Liquid Materials, Journal of Physics: Condensed Matter, Vol. 27, No. 13, 2015, pp. 133201, https://doi.org/10.1088/0953-8984/27/13/133201.
[8] Q. Mei, S. Sinogeikin, G. Shen, S. Amin, C. J. Benmore, K. Ding, High-pressure X-ray Diffraction Measurements on Vitreous GeO₂ under Hydrostatic Conditions, Physical Review B, Vol. 81, No. 17, 2010, pp. 174113, https://doi.org/10.1103/PhysRevB.81.174113.
[9] J. W. E. Drewitt, P. S. Salmon, A. C. Barnes, S. Klotz, H. E. Fischer, W. A. Crichton, Structure of GeO₂ Glass at Pressures up to 8.6 GPa, Physical Review B, Vol. 81, No. 1, 2010, pp. 014202, https://doi.org/10.1103/PhysRevB.81.014202.
[10] G. Lelong, L. Cormier, G. Ferlat, V. Giordano, G. S. Henderson, A. Shukla, G. Calas, Evidence of Fivefold-coordinated Ge Atoms in Amorphous GeO₂ under Pressure, Physical Review B, Vol. 85, No. 13, 2012, pp. 134202, https://doi.org/10.1103/PhysRevB.85.134202.
[11] C. Shi, O. L. G. Alderman, D. Berman, J. Du, J. Neuefeind, A. Tamalonis, J. K. R. Weber, J. You, C. J. Benmore, The Structure of Amorphous and Deeply Supercooled Liquid Alumina, Frontiers in Materials, Vol. 6, 2019,
pp. 38, https://doi.org/10.3389/fmats.2019.00038.
[12] A. F. Harper, K. Iwanowski, W. C. Witt, M. C. Payne, M. Simoncelli, Vibrational and Thermal Properties of Amorphous Alumina from First Principles, Physical Review Materials, Vol. 8, No. 4, 2024, pp. 043601, https://doi.org/10.1103/PhysRevMaterials.8.043601.
[13] W. Li, Y. Ando, S. Watanabe, Effects of Density and Composition on the Properties of Amorphous Alumina: A High-Dimensional Neural Network Potential Study, the Journal of Chemical Physics, Vol. 153, No. 16, 2020,
pp. 164119, https://doi.org/10.1063/5.0026289.
[14] Florian, D. Massiot, B. Poe, I. Farnan, J. P. Coutures, A Time Resolved ²⁷Al NMR Study of the Cooling Process of Liquid Alumina from 2450 °C to Crystallisation, Solid State Nuclear Magnetic Resonance, Vol. 5, No. 4, 1995, pp. 233-238, https://doi.org/10.1016/0926-2040(95)01188-X.
[15] D. R. Neuville, D. de Ligny, L. Cormier, G. S. Henderson, J. Roux, A. Flank, The Crystal and Melt Structure of Spinel and Alumina at High Temperature: an In-situ XANES Study at the Al and Mg K-edges, Geochimica et Cosmochimica Acta, Vol. 73, No. 11, 2009, pp. 3410-3422, https://doi.org/10.1016/j.gca.2009.02.033.
[16] S. K. Lee, S. Ryu, Probing of Triply Coordinated Oxygen in Amorphous Al₂O₃, The Journal of Physical Chemistry Letters, Vol. 9, No. 1, 2018, pp. 150-156, https://doi.org/10.1021/acs.jpclett.7b03027.
[17] F. Harper, S. P. Emge, P. C. M. M. Magusin, C. P. Grey, A. J. Morris, Modelling Amorphous Materials Via a Joint Solid-state NMR and X-ray Absorption Spectroscopy and DFT Approach: Application to Alumina, Chemical Science, Vol. 14, No. 5, 2023, pp. 1155-1167, https://doi.org/10.1039/D2SC04035B.
[18] P. Lamparter, R. Kniep, Structure of Amorphous Al₂O₃, Physica B: Condensed Matter, Vol. 234-236, 1997,
pp. 405-406, https://doi.org/10.1016/S0921-4526(96)01044-7.
[19] H. Hashimoto, Y. Onodera, S. Tahara, S. Kohara, K. Yazawa, H. Segawa, M. Murakami, K. Ohara, Structure of Alumina Glass, Scientific Reports, Vol. 12, 2022, pp. 516, https://doi.org/10.1038/s41598-021-04455-6.
[20] M. Hemmati, M. Wilson, P. A. Madden, Structure of Liquid Al₂O₃ from a Computer Simulation Model, The Journal of Physical Chemistry B, Vol. 103, No. 20, 1999, pp. 4023-4028, https://doi.org/10.1021/jp983529f.
[21] D. J. Lacks, First-Order Amorphous-Amorphous Transformation in Silica, Physical Review Letters, Vol. 84,
No. 20, 2000, pp. 4629-4632, https://doi.org/10.1103/PhysRevLett.84.4629.
[22] V. V. Hoang, Structure and Dynamics of Liquid and Amorphous Al₂O₃·2SiO₂, The European Physical Journal Applied Physics, Vol. 33, No. 1, 2006, pp. 69-76, https://doi.org/10.1051/epjap:2006137.
[23] L. B. Skinner, A. C. Barnes, P. S. Salmon, L. Hennet, H. E. Fischer, C. J. Benmore et al., Joint Diffraction and Modeling Approach to the Structure of Liquid Alumina, Physical Review B, Vol. 87, No. 2, 2013, pp. 024201, https://doi.org/10.1103/PhysRevB.87.024201.
[24] V. V. Hoang, About an Order of Liquid–liquid Phase Transition in Simulated Liquid Al₂O₃, Physics Letters A,
Vol. 335, No. 5-6, 2005, pp. 439-443, https://doi.org/10.1016/j.physleta.2004.12.040.
[25] V. V. Hoang, S. K. Oh, Simulation of Pressure-induced Structural Transformation in Liquid and Amorphous Al₂O₃, Physical Review B, Vol. 72, No. 5, 2005, pp. 054209, https://doi.org/10.1103/PhysRevB.72.054209.
[26] P. K. Hung, T. Vinh, Local Microstructure of Liquid and Amorphous Al₂O₃, Journal of Non-Crystalline Solids, Vol. 352, No. 52-54, 2006, pp. 5531-5540, https://doi.org/10.1016/j.jnoncrysol.2006.09.016.
[27] G. Gutierrez, B. Johansson, Molecular Dynamics Study of Structural Properties of Amorphous Al₂O₃, Physical Review B, Vol. 65, No. 10, 2002, pp. 104202, https://doi.org/10.1103/PhysRevB.65.104202.
[28] X. Zhou, Y. Zhou, Y. Deng, Y. Zhang, Structural, Vibrational and Transport Properties of Liquid and Amorphous Alumina: A Molecular Dynamics Simulation Study, Frontiers in Materials, Vol. 9, 2022, pp. 1005747, https://doi.org/10.3389/fmats.2022.1005747.
Vol. 2008, 2008, pp. 817829, https://doi.org/10.1155/2008/817829.
[2] Y. Zhao, X. Bian, X. Hou, Viscosity and Fragility of the Supercooled and Superheated Liquids of the Ni₆₀Zr₃₀Al₁₀ Metallic Glass-forming Alloy, Physica A: Statistical Mechanics and its Applications, Vol. 367(C), 2006,
pp. 42-54, https://doi.org/10.1016/j.physa.2005.11.020.
[3] K. S. Shamala, L. C. S. Murthy, M. C. Radhakrishna, K. N. Rao, Characterization of Al₂O₃ thin Films Prepared by Spray Pyrolysis Method for Humidity Sensor, Sensors and Actuators A: Physical, Vol. 135, No. 2, 2007,
pp. 552-557, https://doi.org/10.1016/j.sna.2006.10.004.
[4] J. H. Park, T. Suzuki, M. Kurosawa, M. Miyao, T. Sadoh, Nucleation-Controlled Gold-Induced-Crystallization for Selective Formation of Ge(100) and (111) on Insulator at Low-Temperature (~250 °C), Applied Physics Letters, Vol. 103, No. 8, 2013, pp. 082102, https://doi.org/10.1063/1.4819015.
[5] Y. N. Novikov, V. A. Gritsenko, K. A. Nasyrov, Charge Transport Mechanism in Amorphous Alumina, Applied Physics Letters, Vol. 94, No. 22, 2009, pp. 222904, https://doi.org/10.1063/1.3151861.
[6] I. Jackson, Melting of the Silica Isotopes SiO₂, BeF₂ and GeO₂ at Elevated Pressures, Physics of the Earth and Planetary Interiors, Vol. 13, No. 3, 1976, pp. 218–231, https://doi.org/10.1016/0031-9201(76)90096-0.
[7] P. S. Salmon, A. Zeidler, Networks under Pressure: the Development of in Situ High-Pressure Neutron Diffraction for Glassy and Liquid Materials, Journal of Physics: Condensed Matter, Vol. 27, No. 13, 2015, pp. 133201, https://doi.org/10.1088/0953-8984/27/13/133201.
[8] Q. Mei, S. Sinogeikin, G. Shen, S. Amin, C. J. Benmore, K. Ding, High-pressure X-ray Diffraction Measurements on Vitreous GeO₂ under Hydrostatic Conditions, Physical Review B, Vol. 81, No. 17, 2010, pp. 174113, https://doi.org/10.1103/PhysRevB.81.174113.
[9] J. W. E. Drewitt, P. S. Salmon, A. C. Barnes, S. Klotz, H. E. Fischer, W. A. Crichton, Structure of GeO₂ Glass at Pressures up to 8.6 GPa, Physical Review B, Vol. 81, No. 1, 2010, pp. 014202, https://doi.org/10.1103/PhysRevB.81.014202.
[10] G. Lelong, L. Cormier, G. Ferlat, V. Giordano, G. S. Henderson, A. Shukla, G. Calas, Evidence of Fivefold-coordinated Ge Atoms in Amorphous GeO₂ under Pressure, Physical Review B, Vol. 85, No. 13, 2012, pp. 134202, https://doi.org/10.1103/PhysRevB.85.134202.
[11] C. Shi, O. L. G. Alderman, D. Berman, J. Du, J. Neuefeind, A. Tamalonis, J. K. R. Weber, J. You, C. J. Benmore, The Structure of Amorphous and Deeply Supercooled Liquid Alumina, Frontiers in Materials, Vol. 6, 2019,
pp. 38, https://doi.org/10.3389/fmats.2019.00038.
[12] A. F. Harper, K. Iwanowski, W. C. Witt, M. C. Payne, M. Simoncelli, Vibrational and Thermal Properties of Amorphous Alumina from First Principles, Physical Review Materials, Vol. 8, No. 4, 2024, pp. 043601, https://doi.org/10.1103/PhysRevMaterials.8.043601.
[13] W. Li, Y. Ando, S. Watanabe, Effects of Density and Composition on the Properties of Amorphous Alumina: A High-Dimensional Neural Network Potential Study, the Journal of Chemical Physics, Vol. 153, No. 16, 2020,
pp. 164119, https://doi.org/10.1063/5.0026289.
[14] Florian, D. Massiot, B. Poe, I. Farnan, J. P. Coutures, A Time Resolved ²⁷Al NMR Study of the Cooling Process of Liquid Alumina from 2450 °C to Crystallisation, Solid State Nuclear Magnetic Resonance, Vol. 5, No. 4, 1995, pp. 233-238, https://doi.org/10.1016/0926-2040(95)01188-X.
[15] D. R. Neuville, D. de Ligny, L. Cormier, G. S. Henderson, J. Roux, A. Flank, The Crystal and Melt Structure of Spinel and Alumina at High Temperature: an In-situ XANES Study at the Al and Mg K-edges, Geochimica et Cosmochimica Acta, Vol. 73, No. 11, 2009, pp. 3410-3422, https://doi.org/10.1016/j.gca.2009.02.033.
[16] S. K. Lee, S. Ryu, Probing of Triply Coordinated Oxygen in Amorphous Al₂O₃, The Journal of Physical Chemistry Letters, Vol. 9, No. 1, 2018, pp. 150-156, https://doi.org/10.1021/acs.jpclett.7b03027.
[17] F. Harper, S. P. Emge, P. C. M. M. Magusin, C. P. Grey, A. J. Morris, Modelling Amorphous Materials Via a Joint Solid-state NMR and X-ray Absorption Spectroscopy and DFT Approach: Application to Alumina, Chemical Science, Vol. 14, No. 5, 2023, pp. 1155-1167, https://doi.org/10.1039/D2SC04035B.
[18] P. Lamparter, R. Kniep, Structure of Amorphous Al₂O₃, Physica B: Condensed Matter, Vol. 234-236, 1997,
pp. 405-406, https://doi.org/10.1016/S0921-4526(96)01044-7.
[19] H. Hashimoto, Y. Onodera, S. Tahara, S. Kohara, K. Yazawa, H. Segawa, M. Murakami, K. Ohara, Structure of Alumina Glass, Scientific Reports, Vol. 12, 2022, pp. 516, https://doi.org/10.1038/s41598-021-04455-6.
[20] M. Hemmati, M. Wilson, P. A. Madden, Structure of Liquid Al₂O₃ from a Computer Simulation Model, The Journal of Physical Chemistry B, Vol. 103, No. 20, 1999, pp. 4023-4028, https://doi.org/10.1021/jp983529f.
[21] D. J. Lacks, First-Order Amorphous-Amorphous Transformation in Silica, Physical Review Letters, Vol. 84,
No. 20, 2000, pp. 4629-4632, https://doi.org/10.1103/PhysRevLett.84.4629.
[22] V. V. Hoang, Structure and Dynamics of Liquid and Amorphous Al₂O₃·2SiO₂, The European Physical Journal Applied Physics, Vol. 33, No. 1, 2006, pp. 69-76, https://doi.org/10.1051/epjap:2006137.
[23] L. B. Skinner, A. C. Barnes, P. S. Salmon, L. Hennet, H. E. Fischer, C. J. Benmore et al., Joint Diffraction and Modeling Approach to the Structure of Liquid Alumina, Physical Review B, Vol. 87, No. 2, 2013, pp. 024201, https://doi.org/10.1103/PhysRevB.87.024201.
[24] V. V. Hoang, About an Order of Liquid–liquid Phase Transition in Simulated Liquid Al₂O₃, Physics Letters A,
Vol. 335, No. 5-6, 2005, pp. 439-443, https://doi.org/10.1016/j.physleta.2004.12.040.
[25] V. V. Hoang, S. K. Oh, Simulation of Pressure-induced Structural Transformation in Liquid and Amorphous Al₂O₃, Physical Review B, Vol. 72, No. 5, 2005, pp. 054209, https://doi.org/10.1103/PhysRevB.72.054209.
[26] P. K. Hung, T. Vinh, Local Microstructure of Liquid and Amorphous Al₂O₃, Journal of Non-Crystalline Solids, Vol. 352, No. 52-54, 2006, pp. 5531-5540, https://doi.org/10.1016/j.jnoncrysol.2006.09.016.
[27] G. Gutierrez, B. Johansson, Molecular Dynamics Study of Structural Properties of Amorphous Al₂O₃, Physical Review B, Vol. 65, No. 10, 2002, pp. 104202, https://doi.org/10.1103/PhysRevB.65.104202.
[28] X. Zhou, Y. Zhou, Y. Deng, Y. Zhang, Structural, Vibrational and Transport Properties of Liquid and Amorphous Alumina: A Molecular Dynamics Simulation Study, Frontiers in Materials, Vol. 9, 2022, pp. 1005747, https://doi.org/10.3389/fmats.2022.1005747.