Molecular Dynamics and Structural Analysis on the Chemical Strengthening Properties and Impact Resistance of Sodium Alumino-Silicate Glasses

국문 초록 (Abstract)

화학 강화 유리는 유리 매트릭스 내의 Na+ 이온과 용융 염 내의 K+ 이온 간의 이온 교환을 통해 표면에 유도된 압축 응력으로 인해 파괴 강도가 향상됩니다. 나트륨 알루미노실리케이트(SAS) 유리는 전형적인 화학 강화 유리 재료로서 모바일 디스플레이 응용 분야의 시장 수요가 증가함에 따라 광범위한 연구가 수행되었습니다. 본 연구진은 이전연구를 통해 B2O3 및 P2O5와 같은 망목형성체가 도입될 때 SAS 유리의 화학 강화 특성인 압축 응력(CS)과 층의 깊이(DOL)가 변화되었습니다. 이러한 CS 및 DOL의 변화는 B2O3 및 P2O5가 치환 첨가 시 구조적 변화가 발생하며 이를 통한 화학 강화 특성 변화를 유도합니다. 그러나 B2O3 및 P2O5 함량에 따른 구조 변화 및 이에 대한 영향을 설명하는 적절한 연구가 제안되지 않았습니다. 본 연구에서는 분자 동역학(MD) 시뮬레이션을 사용하여 B2O3 및 P2O5 치환 첨가 시 SAS 유리의 구조 변화를 시뮬레이션 하였습니다. 시뮬레이션을 위한 상호 원자 간 포텐셜은 이전 연구들을 통해 얻어진 결과를 사용하여 B2O3 및 P2O5가 포함된 SAS 유리의 유리 내 구조 변화와 화학적 결합을 이해하는 데 중요한 지표인 원자 간 결합 길이, 결합 각도 분포, 배위 수 변화 및 Na+-K+ 이온 간 상호 확산 계수를 계산했습니다. 또한, 실증적 구조 분석으로 Solid-state NMR을 추가적으로 모니터링하였으며 MD 결과와 비교하여 CS 및 DOL에 미치는 영향이 논의되었습니다.
또한, Li2O, K2O, MgO 및 CaO 와 같은 알칼리 및 알칼리 토금속 산화물의 망목변형제 치환 첨가 시 알루미노실리케이트 유리 내 구조 변화와 화학적 강화 특성에 미치는 영향을 밝힐 수 있는 종합적인 연구는 제안된 바 없습니다. 본 연구에서는 추가적으로 앞선 우수한 화학강화 특성을 보인 SiO2-Na2O-Al2O3-P2O5 유리에서 Na2O과 알칼리 및 알칼리 토금속 산화물(Li2O, K2O, MgO 및 CaO)의 다양한 함량을 치환 첨가하여 SAS 유리를 준비하고 CS와 DOL의 변화를 실제 관찰하였습니다. 이러한 조성 변화에 따른 CS 및 DOL의 변화와 구조적 변화 간 상관관계 해석을 위해 Solid-state NMR 및 분자 동역학(MD) 시뮬레이션을 통해 수행된 구조 분석에 의해 설명하고자 하였습니다. 각 구성 요소의 원자 간 결합 길이, 결합 각도 분포, 배위 수 변화 및 Na+-K+ 이온 간 상호 확산 계수를 계산되고 논의되었으며, SAS 유리의 다양한 망목변형제 첨가에 따른 화학적 강화 특성에 대한 새로운 통찰력을 제공했습니다.
마지막으로, 초박형 유리(UTG)는 최근 폴더블 제품에서 핵심 구성 요소입니다. 이에 화학적 강화로 알려진 나트륨 알루미노실리케이트(SAS) 유리는 초박형, 초경량의 커버소재로서 사용되고 있습니다. 이러한 플렉서블 전자 제품에 대한 커버소재 연구는 제품의 수명을 위해 향상된 내구성 및 기계적 강도 연구가 필요합니다. UTG는 50 µm 미만일 때 펜 드롭과 같은 스트레스를 견뎌야 하며, 유리 구조 내에서 충격 시 균열 생성 전에 밀도 증가, 조정 변화 및 전단 흐름 등의 다양한 메커니즘을 통한 충격 에너지를 효과적으로 소산시켜야 합니다. 그러나, 현재까지도 기계적 강도와 구조적 변화 간 메커니즘은 아직 완전히 규명되지 않았습니다. 따라서, 본 연구진은 최근 상업적인 UTG보다 충격 저항성이 크게 향상된 새로운 나트륨 알루미노실리케이트 기반 UTG를 개발했습니다. 분자 동역학(MD) 시뮬레이션과 Solid-state NMR, Micro-Raman, XPS 등의 구조 분석을 사용하여 내충격과 구조적 변화 간 상관관계를 해석하고자 하였습니다. 이러한 UTG 조성의 원자 간 결합 길이, 결합 각도 분포 및 배위 수 변화 계산되고 논의되었으며 UTG의 내충격 메커니즘을 논의하였습니다.

목차 (Table of Contents)

• Table of Contents Ⅰ
• List of Figures and Table Ⅴ
• 1. General Introduction 1
• 1.1. Research Background 1
• 1.2. Objective and Overview of the Thesis 6
• 2. Theoretical Background and Literature Survey 12
• 2.1. Glass Structure Formation 12
• 2.2. Alumino-Silicate Glass 13
• 2.3. Alumino-Silicate Glass Included with P2O5 19
• 2.4. Alumino-Silicate Glass Included with B2O3 23
• 2.5. Alkali Alumino-Silicate Glass 26
• 2.6. Alkali Earth Alumino-Silicate Glass 30
• 2.7. Solid-State NMR Spectroscopy 35
• 2.8. Raman Spectroscopy 39
• 2.9. X-ray Photoelectron Spectroscopy (XPS) 43
• 2.10. Molecular Dynamics Simulation 46
• 2.10.1. General Theory of Molecular Dynamics 46
• 2.10.2. Molecular Dynamics Method 49
• 2.10.3. Monte Carlo Method 49
• 2.10.4. Potential Model 50
• 2.10.5. Equations of Motion and Their Numerical Analysis 54
• 2.10.6. Temperature and Pressure Control for Simulation 56
• 3. Structural Study of Sodium Aluminosilicate Glasses with Varying B2O3 and P2O5 Contents Using Molecular Dynamics and Empirical Analysis 77
• 3.1. Introduction 77
• 3.2. Experimental Procedure 79
• 3.3. Results and Discussion 85
• 3.4. Conclusion 105
• 4. Alkali and Alkaline Earth Oxides Impact on Sodium Aluminosilicate Glass: Strengthening and Structure Analysis 110
• 4.1. Introduction 110
• 4.2. Experimental Procedure 113
• 4.3. Results and Discussion 118
• 4.4. Conclusion 140
• 5. Simulation and Empirical Study of Impact Resistance in Ultra-Thin Sodium-Aluminosilicate Glass 147
• 5.1. Introduction 147
• 5.2. Experimental Procedure 150
• 5.3. Results and Discussion 159
• 5.4. Conclusion 182
• 6. Conclusions 189
• Abstract 192
• Acknowledgments 194
• Curriculum Vitae 196

참고문헌 (Reference)

1. The structure of glasses, Krebs, H., 5(6), 544-554, , 1966

2. Towards Ultrastrong Glasses, Kühn, U., Rouxel, T., Mauro, J. C., Deubener, J., Wondraczek, L., Eckert, J., Horbach, J., Advanced Materials, 23(39), 4578–4586, , 2011

3. Solid-state NMR spectroscopy, Emsley, L., Ashbrook, S. E., Reif, B., Hong, M., Nature Reviews Methods Primers, 1(1), 2, , 2021

4. Universal potential estimates, Mingione, G., Kuusi, T., 262(10), 4205–4269. https//doi. org/10.1016/j. jfa.2012.02.018, , 2012

5. Aluminium in glasses and melts, Lacy, E. D., 4, 234, , 1963

6. Chemical strengthening of glass, Garfinkel, H. M., Bartholomew, R. F., In Glass science and technology (Vol. 5, pp. 217-270). Elsevier, , 1980

7. X-ray photoelectron spectroscopy, Hollander, J. M., Jolly, W. L., 3(6), 193-200, , 1970

8. Reviews in computational chemistry, Lipkowitz, K. B., Boyd, D. B., Cundari, T. R., 25 Wiley-VCH, , 2007

9. The role of P2O5 in silicate melts, Hess, P. C., Ryerson, F. J., 44(4), 611-624, , 1980

10. Ion exchange for glass strengthening, Gy, R., B, 149(2), 159–165. https//doi. org/10.1016/j. mseb.2007.11.029, , 2008

11. Molecular Dynamics Simulation for All, Dror, R. O., Hollingsworth, S. A., 99(6), 1129-1143, , 2018

12. Transport in glassy fast-ion conductors, Ratner, M. A., Pechenik, A., Whitmore, D. H., Susman, S., 101(1), 54–64. https//doi. org/10.1016/0022-3093(88)90368-7, , 1988

13. Die kristallstruktur von Ba13Al22Si10O66, Gebert, W., 135(1-6), 437-452, , 1972

14. Handbook of X-ray photoelectron spectroscopy, King Jr, R. C., Chastain, J., Perkin-Elmer Corporation, 40, 221, , 1992

15. Relaxation processes of densified silica glass, Martinez, V., Champagnon, B., Martinet, C., de Ligny, D., Cornet, A., 146(9), , 2017

16. Modern Raman spectroscopy: a practical approach, Smith, E., Dent, G., John Wiley Sons, , 2019

17. Zur theorie und systematik der molekularkräfte, London, F., 63(3), 245-279, , 1930

18. The Lennard-Jones potential When (not) to use it, Ramírez-Hinestrosa, S., Wang, X., Frenkel, D., Dobnikar, J., 22(19), 10624–10633. https//doi. org/10.1039/C9CP05445F, , 2020

19. Elastic properties of glasses A multiscale approach, Rouxel, T., C. R. Mecanique, , 2006

20. Multinuclear solid state NMR of inorganic materials, MackenzieKJD, S., 6, , 2002

21. Vibrational decoupling of rings in amorphous solids, Elliott, R. J., Barrio, R. A., Galeener, F. L., Martinez, E., 53(25), 2429, , 1984

22. Solid‐state NMR spectroscopic methods in chemistry, Bitter, H. M. L., Jerschow, A., Laws, D. D., 41(17), 3096-3129, , 2002

23. Ultra-thin glass as a substrate for flexible photonics, Mauro, J. C., Macrelli, G., Varshneya, A. K., 106, 109994, , 2020

24. Free-Volume Model of the Amorphous Phase Glass Transition, Cohen, M. H., Turnbull, D., 34(1), 120–125, , 1961

25. Phosphate speciation in potassium aluminosilicate glasses, Hess, P. C., Gan, H., 77(5-6), 495-506, , 1992

26. The short-range structure of sodium ultraphosphate glasses, Hudgens, J. J., Irwin, A. D., Brow, R. K., Tallant, D. R., Martin, S. W., 177, 221-228, , 1994

27. Structure and dynamics of aluminosilicate glasses and melts, Novikov, A., Doctoral dissertation, Université d'Orléans, , 2017

28. Infrared reflectance investigation of alkali diborate glasses, Chryssikos, G. D., Kamitsos, E. I., Patsis, A. P., 152(2-3), 246-257, , 1993

29. Raman investigation of ring configurations in vitreous silica, Mammone, J. F., Sharma, S. K., Nicol, M. F., 292(5819), 140-141, , 1981

30. Young's modulus and compositional parameters of oxide glasses, Morinaga, K., Inaba, S., Fujino, S., 82(12), 3501-3507, , 1999

31. Accelerating the Design of Functional Glasses through Modeling, Smedskjaer, M. M., Mauro, Y. Z., Mauro, J. C., Vargheese, K. D., Tandia, A., 28(12), 4267 –4277, , 2016

32. Band limits and the vibrational spectra of tetrahedral glasses, Galeener, F. L., Physical Review B, 19(8), 4292, , 1979

33. Structure and mechanical properties of aluminosilicate glasses, Grammes, T., Doctoral dissertation, Dissertation, Jena, Friedrich-Schiller-Universität Jena, , 2020

34. The Nature of the Glass Transition in a Silica-Rich Oxide Melt, Farnan, I., Stebbins, J. F., 265(5176), 1206– 1209. https//doi. org/10.1126/science.265.5176.1206, , 1994

35. Elastic Properties and Short‐to Medium‐Range Order in Glasses, Rouxel, T., 90(10), , 2007

36. Poissons ratio and the densification of glass under high pressure, Hammouda, T., Rouxel, T., Ji, H., Moréac, A., 100(22), 225501, , 2008

37. The physics of chemical strengthening of glass room for a new view, Varshneya, A. K., 356(44-49), 2289-2294, , 2010

38. Viscosity and thermal expansion of lithium aluminosilicate glassesa), Shelby, E., 49(12), , 1978

39. Advances in Raman spectroscopy applied to earth and material sciences, De Ligny, D., Neuville, D. R., Henderson, G. S., 78(1), 509-541, , 2014

40. Chemical strengthening of glass lessons learned and yet to be learned, Varshneya, A. K., 1(2), 131-142, , 2010

41. Structure and properties of low-silica calcium aluminosilicate glasses, Calas, G., Cormier, L., Neuville, D. R., 274(1-3), 110-114, , 2000

42. A new low‐brittleness glass in the soda ‐lime‐silica glass family, Ito, S., Sehgal, J., 81(9), 2485-2488, , 1998

43. Alkali diffusivity in alkaline earth sodium boroaluminosilicate glasses, Potuzak, M., Smedskjaer, M. M., Solid State Ionics, 263, 95–98. https//doi. org/10.1016/j. ssi.2014.05.015, , 2014

44. Bridging and nonbridging oxygen atoms in alkali aluminosilicate glasses, Tasker, G. W., Uhlmann, D. R., Struck, C. W., Alexander, M. N., Onorato, P. I., 68(6), C-148, , 1985

45. Local Al site distribution in aluminosilicate glasses by 27Al MQMAS NMR, Massiot, D., Montouillout, V., Neuville, D. R., Cormier, L., 353(2), 180-184, , 2007

46. NMR evidence for excess non-bridging oxygen in an aluminosilicate glass, Xu, Z., Stebbins, J. F., 390(6655), 60-62, , 1997

47. Characterization of alkali silica reaction gels using Raman spectroscopy, Balachandran, C., Muñoz, J. F., Arnold, T., 92, 66-74, , 2017

48. Development of empirical potentials for sodium borosilicate glass systems, Cormier, L., Stolz, C., Delaye, J. M., Kieu, L. H., 357(18), 3313–3321. https//doi. org/10.1016/j. jnoncrysol.2011.05.024, , 2011

49. Elastic interpretation of the glass transition in aluminosilicate liquids, Huang, L., Scannell, G., Mauro, J. C., Smedskjaer, M. M., 85(14), 144203, , 2012

50. Indentation deformation mechanism in glass densification versus shear flow, Rouxel, T., Guin, J. P., Ji, H., Rufflé, B., Augereau, F., 107(9), , 2010

51. Ion‐Exchanged Lithium Aluminosilicate Glass Strength and Dynamic Fatigue, Seaman, J. H., Blanchet, T. A., Tomozawa, M., Lezzi, P. J., Aaldenberg, E. M., 99(8), 2645–2654. https//doi. org/10.1111/jace.14294, , 2016

52. The distribution of aluminum in the tetrahedra of silicates and aluminates, Loewenstein, W., 39(1-2), 92-96, , 1954

53. The mechanical strength of alkali-aluminosilicate glasses after ion exchange, Burggraaf, A. A., Technische Hogeschool Eindhoven. https//doi. org/10.6100/IR95070, , 1965

54. Microscopic Origins of Compositional Trends in Aluminosilicate Glass Properties, Smedskjaer, M. M., Mauro, J. C., Yue, Y., Kjeldsen, J., 96(5), , 2013

55. New interaction potentials for alkali and alkaline-earth aluminosilicate glasses, Kob, W., Ispas, S., Sundararaman, S., Huang, L., 150(15), 154505. https//doi. org/10.1063/1.5079663, , 2019

56. Structure and mechanical properties of compressed sodium aluminosilicate glasses, Bechgaard, T. K., Role of non-bridging oxygens, , 2016

57. The Characterization of Obsidian and its application to the Mediterranean Region, Cann, J. R., Renfrew, C., 30, 111–133, , 1964

58. Chemical Strengthening of Sodium Aluminosilicate Glasses Containing P2O5 and B2O3, Choi, Y. G., Chung, W. J., Park, K. D., Han, K., 554, 120600. https//doi. org/10.1016/j. jnoncrysol.2020.120600, , 2021

59. Molecular dynamics simulation of lithium diffusion in Li2O–Al2O3–SiO2 glasses, Garofalini, S. H., Li, W., Solid State Ionics, , 2004

60. Composition dependence of indentation deformation and indentation cracking in glass, Sellappan, P., Houizot, P., Celarie, F., Rouxel, T., Conradt, R. J. A. M., Becker, E., 61(16), 5949-5965, , 2013

61. Topological hardening through oxygen triclusters in calcium aluminosilicate glasses, Mauro, J. C., Wilkinson, C. J., Bragatto, C. B., Ono, M., Lee, K., Welch, R. S., 104(12), 6183–6193. https//doi. org/10.1111/jace.18032, , 2021

62. Indentation cracking and deformation mechanism of sodium aluminoborosilicate glasses, Smedskjaer, M. M., Januchta, K., Hansen, S. R., To, T., Liu, P., 103(3), 1656-1665, , 2020

63. Local structure of Si and P in SiO2- P2O5 and Na2O- SiO2- P2O5 glasses A XANES study, Kasrai, M., Pan, Y., Fleet, M. E., Bancroft, G. M., Li, D., 188(1-2), 181-189, , 1995

64. Elastic moduli of XAlSiO4 aluminosilicate glasses Effects of charge-balancing cations, Clément, S., Vialla, R., Dupas, C., Rufflé, B., Le Losq, C., Weigel, C., Neuville, D. R., 447, 267–272. https//doi. org/10.1016/j. jnoncrysol.2016.06.023, , 2016

65. Evidence of intermediate-range order heterogeneity in calcium aluminosilicate glasses, Skibsted, J., Moesgaard, M., Keding, R., Yue, Y., 22(15), 4471-4483, , 2010

66. Chemical Composition and Mechanical Properties of Basalt and Glass Fibers A Comparison, Czigány, T., Deák, T., 79(7), 645–651, , 2009

67. Chemical Strengthening of Ultra-Thin Glass for Use as Cover Window of Flexible Displays, Lee, J. I., Ko, S. Y., Choi, Y. G., Ceramist, 25(3), 287–298. https//doi. org/10.31613/ceramist.2022.25.3.06, , 2022

68. Soda-lime silicate glass under hydrostatic pressure and indentation a micro-Raman study, Deschamps, T., Bruneel, J. L., Champagnon, B., Martinet, C., Journal of Physics Condensed Matter, 23(3), 035402, , 2011

69. Structure of sodium sluminosilicate melts containing at least 50 mole % SiO2 at 1500°C, Riebling, E. F., 44(8), 2857–2865. https//doi. org/10.1063/1.1727145, , 1966

70. Ultra-Smooth and Ultra-Strong Ion-Exchanged Glass as Substrates for Organic Electronics, Mauro, J. C., He, M., Pambianchi, M. S., Feng, J., Bao, Z., Käfer, D., Li, J., 23(25), 3233–3238, , 2013

71. Viscosity, fragility, and configurational entropy of melts along the join SiO2-NaAlSiO4, Hess, K.-U., Lenci, T., Dingwell, D. B., Toplis, M. J., 82(9–10), 979–990. https//doi. org/10.2138/am-1997-9-1014, , 1997

72. Structural characterization of lanthanum aluminosilicate glasses by 29Si solid-state NMR, Edén, M., Leonova, E., Iftekhar, S., 355(43–44), 2165–2174. https//doi. org/10.1016/j. jnoncrysol.2009.06.031, , 2009

73. 27 Al and 29 Si NMR study of sol-gel derived aluminosilicates and sodium aluminosilicates, Holmgren, J. S., Jonas, J., Irwin, A. D., 23, 2908-2912, , 1988

74. 6 Chemical strengthening of ultra-thin glass for use as cover window of flexible displays, Ko, S. Y., Choi, Y. G., ceramist, 25(3), 287–298. https//doi. org/10.31613/ceramist.2022.25.3.06, , 2022

75. First-principles calculation of the 17O NMR parameters of a calcium aluminosilicate glass, Pickard, C. J., Profeta, M., Mauri, F., Tuckerman, M. E., Benoit, M., 109(13), 6052-6060, , 2005

76. Fivefold-coordinated aluminum in tectosilicate glasses observed by triple quantum MAS NMR, Poplett, I. J., Smith, M. E., Kohn, S. C., Toplis, M. J., 85(10), 1556-1560, , 2000

77. Synthesis, thermal and structural properties of pure TeO2 glass and zinc-tellurite glasses, Kyritsis, A., Simandiras, E. D., Psycharis, V., Tagiara, N. S., Kamitsos, E. I., Palles, D., 457, 116-125, , 2017

78. 17O 3Q-MAS NMR characterization of a sodium aluminoborosilicate glass and its alteration gel, Charpentier, T., Gin, S., Petit, J. C., Angeli, F., 341(1–2), 23–28. https//doi. org/10.1016/S0009-2614(01)00423-7, , 2001

79. A multi-step chemical ion-exchange process for alkali/alkaline-earth aluminosilicate glasses, Hu, W., Zhang, Y., Tan, B., Chen, F., Tian, Y., Lu, P., Chen, X., Ceramics International, 45(18), 24878–24883. https//doi. org/10.1016/j. ceramint.2019.09.050, , 2019

80. Defect-mediated self-diffusion in calcium aluminosilicate glasses A molecular modeling study, Vargheese, K. D., Tandia, A., Mauro, J. C., Timofeev, N. T., 357(7), 1780-1786, , 2011

81. Development of boron oxide potentials for computer simulations of multicomponent oxide glasses, Du, J., Deng, L., 102(5), 2482–2505. https//doi. org/10.1111/jace.16082, , 2019

82. Molecular dynamics simulations of structural changes in mixed alkali (Li–K) silicate glasses, Cormack, A. N., Park, B., 255(1), 112–121. https//doi. org/10.1016/S0022-3093(99)00430-5, , 1999

83. Structure and properties of sodium aluminosilicate glasses from molecular dynamics simulations, Smedskjaer, M. M., Xiang, Y., Mauro, J. C., Du, J., 139(4), 044507. https//doi. org/10.1063/1.4816378, , 2013

84. Al and Sr environment in tectosilicate glasses and melts viscosity, Raman and NMR investigation, Charpentier, T., Hennet, L., Thiaudière, D., Florian, P., Novikov, A. N., Gueguen, Y., Neuville, D. R., 461, 115-127, , 2017

85. Structure of Mg-and Mg/Ca aluminosilicate glasses 27Al NMR and Raman spectroscopy investigations, Cormier, L., Rifflet, J. C., Florian, P., Neuville, D. R., Massiot, D., Montouillout, V., Millot, F., 93(11-12), 1721-1731., , 2008

86. Structure of calcium aluminosilicate glasses Wide-angle X-ray scattering and computer simulation, Nofz, M., Himmel, B., Weigelt, J., Gerber, Th., 136(1–2), 27–36. https//doi. org/10.1016/0022-3093(91)90115-M, , 1991

87. Understanding the structure and structural effects on the properties of blast furnace slag (BFS), Aamir, M., Yan, Z., You, Z., Lv, X., Sajid, M., Bai, C., ISIJ International, 59(7), 1153–1166. https//doi. org/10.2355/isijinternational. ISIJINT-2018-453, , 2019

88. Young s modulus, Vickers hardness and indentation fracture toughness of alumino silicate glasses, Tiegel, M., Ceramics International, , 2015

89. Site connectivities in sodium aluminoborate glasses multinuclear and multiple quantum NMR results, Du, L. S., Stebbins, J. F., 27(1-2), 37-49, , 2005

90. The structure of alkaline earth aluminosilicate glasses as determined by vibrational spectroscopy, Merzbacher, C. I., White, W. B., 130(1), 18-34, , 1991

91. Ionic conductivity in glasses A Monte-Carlo study of ordered and disordered one-dimensional models, Susman, S., Whitmore, D., Ratner, M., Pechenik, A., 18–19, 403– 409. https//doi. org/10.1016/0167-2738(86)90150-5, , 1986

92. Realizing translucency in aluminosilicate glass at ultralow temperature via cold sintering process, Cheng, X., Wang, K., Jiang, W., Luo, W., Gao, J., Fan, Y., 11(11), 1714-1724, , 2022

93. A theoretical interpretation of the chemical shift of 29Si NMR peaks in alkali borosilicate glasses, Nanba, T., Nishimura, M., Miura, Y., 68(24), 5103-5111, , 2004

94. Ca–Mg mixing in aluminosilicate glasses An investigation using 17O MAS and 3QMAS and 27Al MAS NMR, Allwardt, J. R., Stebbins, J. F., Kelsey, K. E., 354(40-41), 4644-4653, , 2008

95. Quantitative measurement of Q3 species in silicate and borosilicate glasses using Raman spectroscopy, Larson, C., Holland, D., Doerr, J., Affatigato, M., Parkinson, B. G., Smith, M. E., Scales, C. R., 354(17), 1936-1942., , 2008

96. Chemical Strengthening of Glass Lessons Learned and Yet To Be Learned Chemical Strengthening of Glass, Varshneya, A. K., 1(2), 131–142, , 2010

97. Analysis of fracture mechanisms of ultrathin glass for flexible cover window under pen drop conditions, Kim, S., Shim, G., Jung, S., Chung, W. J., Shon, H., Park, K. D., Kim, S., 106(1), 569-581, , 2023

98. Elastic constants, Vickers hardness, and fracture toughness of fluorrichterite-based glass– ceramics, Holloway, J. A., Denry, I. L., 20(3), 213-219, , 2004

99. Structure and the extent of disorder in quaternary (Ca-Mg and Ca-Na) aluminosilicate glasses and melts, Mysen, B. O., Lee, S. K., Cody, G. D., 90(8-9), 1393-1401, , 2005

100. Effects of Thermal and Pressure Histories on the Chemical Strengthening of Sodium Aluminosilicate Glass, Smedskjaer, M. M., Frontiers in Materials 3, , 2016

101. Raman micro‐spectroscopy of western Mediterranean obsidian glass One step towards provenance studies?, Bourdonnec, F. L., Poupeau, G., Dubernet, S., Bellot‐Gurlet, L., 35(8–9), 671–677, , 2004

102. 3 Analysis of fracture mechanisms of ultrathin glass for flexible cover window under pen drop conditions, Shim, G., Park, K. D., Jung, S., Shon, H., Kim, S., Chung, W. J., 106(1), 569–581. https//doi. org/10.1111/jace.18741, , 2023

103. Modeling oxide glasses with Born–Mayer–Huggins potentials Effect of composition on structural changes, Louis-Achille, V., Delaye, J. M., Ghaleb, D., 210(2– 3), 232–242. https//doi. org/10.1016/S0022-3093(96)00604-7, , 1997

104. Structure of Cerium Phosphate Glasses Molecular Dynamics Simulation Structure of Cerium Phosphate Glasses, Chen, Y., Rygel, J. L., Du, J., Woodman, R., Pantano, C. G., Belcher, J., Kokou, L., 94(8), 2393– 2401. https//doi. org/10.1111/j.1551-2916.2011.04514. x, , 2011

105. Molecular dynamics simulation for ligand-receptor studies. Carbohydrates interactions in aqueous solutions, Grigera, J., 8(17), 1579-1604, , 2002

106. Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides, Shannon, R. D., Acta crystallographica section A crystal physics, diffraction, theoretical and general crystallography, 32(5), 751-767, , 1976

107. The role of Al3+ on rheology and structural changes in sodium silicate and aluminosilicate glasses and melts, Losq, C. L., Geochimica et Cosmochimica Acta, , 2014

108. A critical evaluation of indentation techniques for measuring fracture toughness I, direct crack measurements, Chantikul, P., Marshall, D. B., Lawn, B. R., Anstis, G. R., 64(9), 533-538, , 1981

109. Striking role of non-bridging oxygen on glass transition temperature of calcium aluminosilicate glass-formers, Jakse, N., Pasturel, A., Bouhadja, M., 140(23), , 2014

110. High-resolution 29Si NMR study of silicate and aluminosilicate glasses the effect of network-modifying cations, Carmichael, I. S., Stebbins, J. F., Murdoch, J. B., 70(3-4), 332-343, , 1985

111. A modified random network model for P2O5–Na2O–Al2O3– SiO2 glass studied by molecular dynamics simulations, Cao, X., Zhao, Y., Han, G., Zhang, C., Qiao, X., Du, J., Xu, G., 11(12), 7025-7036, , 2021

112. An NMR spectroscopic investigation of aluminosilicate gel in alkali-activated fly ash in a CO2-rich environment, Park, S. M., Jang, J. G., Chae, S. A., Lee, H. K., Materials, 9(5), 308, , 2016

113. Polyhedral units and network connectivity in calcium aluminosilicate glasses from high-energy X-ray diffraction, Petkov, V., Himmel, B., Shastri, S. D., Billinge, S. J. L., 85(16), 3436, , 2000

114. A modified random network model for P2O5 – Na2O–Al2O3–SiO2 glass studied by molecular dynamics simulations, Han, G., Peng, S., Du, J., Zhao, Y., Zhang, C., Qiao, X., Cao, X., Xu, G., Liu, Y., 11(12), 7025–7036. https//doi. org/10.1039/D0RA10810C, , 2021

115. Field strength effect on structure, hardness, and crack resistance in single modifier aluminoborosilicate glasses, Fry, A. L., Kim, S. H., George, C., Feller, S., Hawbaker, H., Mauro, J. C., Slagle, I., 106(2), 951– 966. https//doi. org/10.1111/jace.18796, , 2023

116. Nuclear magnetic resonance investigation of the structures of phosphate and phosphate-containing glasses A review, Kirkpatrick, R. J., Solid State Nuclear Magnetic Resonance, , 1995

117. Density and Young s Modulus of ternary glasses close to the eutectic composition in the CaO–Al2O3– SiO2-system, Rüssel, C., Veit, U., Ceramics International, 42(5), 5810-5822, , 2016

118. A thermochemical study of glasses and crystals along the joins silica-calcium aluminate and silica-sodium aluminate, McMillan, P., Peraudeau, G., Coutures, J. P., Navrotsky, A., 46(11), 2039-2047, , 1982

119. Correlation between K+-Na+ diffusion coefficient and flexural strength of chemically tempered aluminosilicate glass, Li, X., Mohagheghian, I., Li, L., Jiang, L., Yan, Y., Dear, J. P., Wang, Y., 471, 72–81. https//doi. org/10.1016/j. jnoncrysol.2017.05.011, , 2017

120. Effect of modifier cation field strength on the structures of magnesium oxide containing aluminoborosilicate glasses, Tuheen, M. I., Du, J., 13(4), 554–567. https//doi. org/10.1111/ijag.16599, , 2022

121. Molecular dynamics study of the structural properties of calcium aluminosilicate slags with varying Al2O3/SiO2 ratios, Zheng, K., Sridhar, S., Zhang, Z., Yang, F., ISIJ international, 52(3), 342-349, , 2012

122. Structure and crystallization of alkaline-earth aluminosilicate glasses prevention of the alumina-avoidance principle, Siegel, R., Mather, G. C., Ganisetti, S., Allu, A. R., Ferreira, J. M., Gaddam, A., Balaji, S., 122(17), 4737-4747., , 2018

123. Molecular dynamic simulations study on the structure and properties of Li2O-containing magnesium aluminosilicate glasses, Zhong, C., Huang, S., Chen, C., Zu, Q., Li, A., Zhang, Y., Zeng, H., 32, 103945. https//doi. org/10.1016/j. mtcomm.2022.103945, , 2022

124. Temperature effects on non-bridging oxygen and aluminum coordination number in calcium aluminosilicate glasses and melts, Stebbins, J. F., Kelsey, K. E., Dubinsky, E. V., Kanehashi, K., 72(3), 910-925, , 2008

125. Atomistic insights into the impact of charge balancing cations on the structure and properties of aluminosilicate glasses, Hasnaoui, A., Ghardi, E. M., Ouaskit, S., 17 Physical Review B, 100(14), 144109. https//doi. org/10.1103/PhysRevB.100.144109, , 2019

126. Structural behavior of Al3+ in peralkaline, metaluminous, and peraluminous silicate melts and glasses at ambient pressure, Toplis, M. J., Mysen, B. O., 92(5-6), 933-946, , 2007

127. Molecular dynamics simulations of the structural properties and electrical conductivities of CaO–MgO–Al2O3–SiO2 melts, Venter, G. A., Mongalo, L., Lopis, A. S., 452, 194-202, , 2016

128. Phosphorus solubility mechanisms in haplogranitic aluminosilicate glass and melt Effect of temperature and aluminum content, Mysen, B. O., 133(1), 38-50, , 1998

129. Effect of alkali and alkaline-earth metal oxides on the chemical strengthening properties of sodium alumino-silicate glasses, Park, K. D., Jeong, B.-Y., Gelija, D., Chung, W. J., 625, 122769, , 2024

130. Effect of alkali and alkaline-earth metal oxides on the chemical strengthening properties of sodium alumino-silicate glasses, Jeong, B.-Y., Gelija, D., Chung, W. J., 625, 122769. https//doi. org/10.1016/j. jnoncrysol.2023.122769, , 2024

131. Properties of Soda Aluminosilicate Glasses I, Refractive Index, Density, Molar Refractivity, and Infrared Absorption Spectra, Day, D. E., Rindone, G. E., 45(10), 489–496. https//doi. org/10.1111/j.1151-2916.1962. tb11040. x, , 1962

132. Mechanical–Structural Investigation of Chemical Strengthening Aluminosilicate Glass through Introducing Phosphorus Pentoxide, Yang, B., Wang, L., Ye, F., Chen, J., Sun, L., Chen, G., Zeng, H., Frontiers in Materials, 3. https//doi. org/10.3389/fmats.2016.00053, , 2016

133. New Glass Technologies for Enhanced Architectural Surety Engineered Stress Profiles in Soda-Lime-Silica Glass (No. SAND2000-3001), Abrams, M., Glass, S. J., Matalucci, R. V., Sandia National Lab.(SNL-NM), Albuquerque, NM (United States); Sandia National Lab.(SNL-CA), Livermore, CA (United States)., , 2000

134. Al speciation and Ca environment in calcium aluminosilicate glasses and crystals by Al and Ca K-edge X-ray absorption spectroscopy, Briois, V., Cormier, L., Massiot, D., Neuville, D. R., Flank, A. M., 213(1-3), 153-163, , 2004

135. Effects of the degree of polymerization on the structure of sodium silicate and aluminosilicate glasses and melts An 17O NMR study, Stebbins, J. F., Lee, S. K., Geochimica et Cosmochimica Acta, 73(4), 1109–1119. https//doi. org/10.1016/j. gca.2008.10.040, , 2009

136. Alumina effect on the structure and properties of calcium aluminosilicate in the percalcic region A molecular dynamics investigation, Atila, A., Hasnaoui, A., Ouaskit, S., Ghardi, E. M., 525, 119470, , 2019

137. Structural, thermal, and optical analysis of zinc boro-aluminosilicate glasses containing different alkali and alkaline modifier ions, Lakshminarayana, G., Kaky, K. M., Baki, S. O., Kityk, I. V., Taufiq-Yap, Y. H., Mahdi, M. A., Journal of Non-Crystalline Solids, 456, 55-63., , 2017

138. Environments of Mg and Al in MgO–Al2O3–SiO2 glasses A study coupling neutron and X-ray diffraction and Reverse Monte Carlo modeling, Guignard, M., Cormier, L., 256(3-4), 111-118, , 2008

139. Al coordination and speciation in calcium aluminosilicate glasses Effects of composition determined by 27Al MQ-MAS NMR and Raman spectroscopy, Massiot, D., Cormier, L., Neuville, D. R., 229(1-3), 173-185, , 2006

140. Bulk structures of silica-rich calcium aluminosilicate (CAS) glasses along the molar CaO/Al2O3= 1 join via molecular dynamics (MD) simulation, Cormack, A. N., LaCourse, W., Lamberson, L., Agnello, G., Youngman, R., Smith, N., 519, 119450., , 2019

141. Bonding preferences of non-bridging O atoms Evidence from 17O MAS and 3QMAS NMR on calcium aluminate and low-silica Ca-aluminosilicate glasses, Keun Lee, S., Allwardt, J. R., Stebbins, J. F., 88(7), 949-954, , 2003

142. Non-stoichiometric non-bridging oxygens and five-coordinated aluminum in alkaline earth aluminosilicate glasses Effect of modifier cation size, Stebbins, J. F., Thompson, L. M., 358(15), 1783-1789, , 2012

143. Development of effective empirical potentials for molecular dynamics simulations of the structures and properties of boroaluminosilicate glasses, Du, J., Deng, L., 453, 177–194. https//doi. org/10.1016/j. jnoncrysol.2016.09.021, , 2016

144. Structure− property relations in mixed-network glasses multinuclear solid state NMR investigations of the system x Al2O3(30 − x) P2O5 70SiO2, Aitken, B. G., Youngman, R. E., Eckert, H., Deshpande, R. R., 113(8), 3322-3331., , 2009

145. Thermochemistry of Charge ‐Coupled Substitutions in Silicate Glasses The Systems Ml/nn+ AlO2‐SiO2 (M= Li, Na, K, Rb, Cs, Mg, Ca, Sr, Ba, Pb), NAVROTSKY, A., Roy, B. N., 67, , 1984

146. Structural studies of calcium aluminosilicate glasses by high resolution solid state 29Si and 27Al magic angle spinning nuclear magnetic resonance, Engelhardt, G., 26, 157-165, , 1985

147. Silicate-phosphate interactions in silicate glasses and melts II. quantitative, high-temperature structure of P-bearing alkali aluminosilicate melts, Mysen, B. O., Cody, G. D., 65(14), 2413–2431. https//doi. org/10.1016/S0016-7037(01)00598-1, , 2001

148. Relationship Between Structure and Glass Transition Temperature in Low‐silica Calcium Aluminosilicate Glasses The Origin of the Anomaly at Low Silica Content, Cormier, L., Calas, G., Neuville, D. R., 88(8), 2292– 2299. https//doi. org/10.1111/j.1551-2916.2005.00428. x, , 2005

149. Characterization of the structure of calcium alumino-silicate and calcium fluoro-alumino-silicate glasses by magic angle spinning nuclear magnetic resonance (MAS-NMR), Hill, R. G., Stamboulis, A., Law, R. V., 333(1), 101-107, , 2004

150. Probing silicon and aluminium chemical environments in silicate and aluminosilicate glasses by solid state NMR spectroscopy and accurate first-principles calculations, Menziani, M. C., Gambuzzi, E., Charpentier, T., Caurant, D., Angeli, F., Pedone, A., 125, , 2014

151. Mixed network former effect on structure, physical properties, and bioactivity of 45S5 bioactive glasses An integrated experimental and molecular dynamics simulation study, Thomas, T., Du, J., Deng, L., Chen, J., Huntley, C., Ren, M., Kuo, P.-H., Lu, X., 122(9), 2564–2577. https//doi. org/10.1021/acs. jpcb.7b12127, , 2018

152. Mixed network former effect on structure, physical properties, and bioactivity of 45S5 bioactive glasses an integrated experimental and molecular dynamics simulation study, Huntley, C., Lu, X., Thomas, T., Ren, M., Du, J., Deng, L., Kuo, P. H., 122(9), 2564-2577., , 2018