硅酸盐学报

化学计量碱金属二硅酸盐玻璃-晶体界面能的分子动力学研究：基于晶体最小能量切割法

PDF下载

Chandra Saha LETON , Murata TETSUYA , Nakane SHINGO

硅酸盐学报 | 先进玻璃与光学材料专题——研究论文 2025,54(4): 1291-1298

收起

硅酸盐学报 | 先进玻璃与光学材料专题——研究论文 2025, 54(4): 1291-1298

化学计量碱金属二硅酸盐玻璃-晶体界面能的分子动力学研究：基于晶体最小能量切割法

全屏

Chandra Saha LETON, Murata TETSUYA, Nakane SHINGO

作者信息

日本电气硝子株式会社基础技术事业部，滋贺县大津市 520-8639，日本

LETON Chandra Saha（1980—），男，博士，主任研究员。

LETON Chandra Saha (1980-), male, Ph.D, Senior researcher. E-mail: lsaha@neg.co.jp

Molecular Dynamics Studies of Interfacial Energy in Stochiometric Alkali Disilicate Glass-Crystals Based on Crystal Minimum Energy Cutting

Chandra Saha LETON, Murata TETSUYA, Nakane SHINGO

Affiliations

Fundamental Technology Division, Nippon Electric Glass, Otsu 520-8639, Shiga, Japan

出版时间: 2025-11-10 doi: 10.14062/j.issn.0454-5648.20250430

文章导航

摘要

收起

为估算玻璃与晶体之间的界面能（σ），基于Tielemann理论，采用分子动力学模拟开发了一种晶体最小能量切割界面模型。使用该模型可复现实验测得的化学计量碱金属二硅酸盐（如Li₂O·2SiO₂、Na₂O·2SiO₂与K₂O·2SiO₂）玻璃-晶体体系中界面能规律，即σ_Li > σ_Na > σ _K。进一步通过分析界面配位数（CN_int），推导出键强-配位数关系，该关系与界面能存在内在关联。

关键词

玻璃-晶体界面能 / 分子动力学模拟 / 原子间势函数 / 界面配位数

Abstract

收起

Introduction

Crystallization control is crucial during glass production. In glass crystallization theory, it has been hypothesized that there is a direct relationship between glass-crystal interfacial energy and nucleation rate. Since it is difficult to measure interfacial energy directly, classical nucleation theory is used to obtain it. However, the estimation process is complex; various measurement data such as the nucleation rate, viscosity, and Gibbs free energy barriers between the glass and crystal are required. Overall, estimating the glass-crystal interfacial energy is time-consuming. In this regard, the interfacial energy can be directly obtained using molecular dynamics (MD) simulations. In this study, we implemented an interface model to estimate the glass-crystal interfacial energy based on the theory of Tielemann et al., which was recently introduced to generate crystal orientation planes using minimum-energy cuts. To the best of our knowledge, this is the first work in which the crystal orientation plane determined based on a minimum-energy cutting process has been used to build a glass-crystal interface in a more realistic environment (i.e., hypothesizes that a minimum-energy structure may occur during crystal nucleation) and calculate the interfacial energy. To achieve this, we considered stoichiometric alkali (Li, Na, and K) disilicate (2SiO₂) glasses and crystals, as some early-stage experimental data have been reported, which are highly beneficial for validating the MD results. The effects of different potential models were also investigated and found that they had a significant impact on the reproduction of the experimental trend.

Methods

Simulations were performed using the LAMMPS package. The temperature and pressure were controlled with the Nose-Hoover thermostat and barostat, respectively. After setting up the glass-crystal interface using NPT, we ran MD simulations with NVT for another 200 ps to calculate the interfacial energy. The MD simulations were performed with a time step of 1 fs. Periodic boundary conditions were applied in all directions. Cutoff distances were applied according to references. We used three interatomic potential (SHIK, Du, and Pedone) models to estimate the interfacial energies of Li₂O-2SiO₂ glass-Li₂O-2SiO₂ (001), Na₂O-2SiO₂ glass-Na₂O-2SiO₂ (010), and K₂O-2SiO₂ glass-K₂O-2SiO₂ (001). All three of these potential functions are widely used. The glass structure was fabricated from the crystal structures by simulating a melt-quenching process. First, the Li₂O-2SiO₂ (001), Na₂O-2SiO₂ (010), and K₂O-2SiO₂ (001) crystal structures were prepared. Half the crystal was kept fixed, while the other half was melted at 3500 K with a canonical ensemble (NVT) for 300 ps and then quenched to 300 K at a cooling rate of 5 K/ps. After the melt-quenching process, the crystal part was unfixed and relaxed for 200 ps with a glassy structure using an isobaric-isothermal ensemble (NPT) at a temperature of 300 K. An interfacial model was developed by the theory of Tielemann et al, where the crystal plane was determined through the minimum energy cut in the crystal structure.

Results and discussion

We first evaluated the glass density by calculating the local density profile along the z-direction of Li₂O-2SiO₂ glass-Li₂O-2SiO₂ (001), Na₂O-2SiO₂ glass-Na₂O-2SiO₂ (010), and K₂O-2SiO₂ glass-K₂O-2SiO₂ (001). The glass structures show density results comparable to the experimental data.

The calculated interfacial energy values using the SHIK potential show a similar experimental trend, while the Du and Pedone potentials are unable to reproduce the experimental trend. However, the potentials of Du and Pedone show better values of interfacial energy for the glass-crystal interface of Li₂O-2SiO₂ than the SHIK. Our MD results demonstrate that among the potential models, SHIK is a good candidate for calculating interfacial energy in terms of experimental reproduction.

We analyzed the interfacial coordination number (i.e., cation-anion) in the contact area between the glass and crystal surfaces. These coordination numbers are difficult to estimate experimentally. Typically, the coordination number is determined in the bulk region of a glass or crystal structure. We found that the interfacial coordination number varies significantly at the glass-crystal interface of Li₂O-2SiO₂, Na₂O-2SiO₂, and K₂O-2SiO₂. Among the interfacial systems, coordination number values of two, three, four, and five were observed, the most frequently observed value was one. The values were significantly lower at four and five for K₂O-2SiO₂and Na₂O-2SiO₂, respectively. Our MD results demonstrated that the cation (Li, Na, and K)-anion environments were not the same in the interfacial domain. For further evaluation, we calculated the bond strength-coordination number.

The bond strength-coordination number has been reported for chalcogenide glasses. In the present work, the bond strength-coordination number is introduced for glass-crystal interface systems. The calculated results of bond strength-coordination number show a decreasing trend in the order Li > Na > K, which is similar to interfacial energy. Overall, analysis revealed that the alkali (Li, Na, and K)—O bond plays a crucial role in the interfacial strength.

Conclusion

We developed an interface model using molecular dynamics simulations based on the minimum energy cut of crystals with glassy structures. The minimum energy cut of the crystal was determined by applying Tielemann theory. The modeled interfaces were between glass and crystals in stoichiometric alkali (Li, Na, and K) disilicates. The interface model reproduced the experimental interfacial energy trend of Li > Na > K; the interatomic potential model was found to have a significant effect on reproduction. The MD results indicate that the SHIK-based MD model could reproduce the experimental results better than the other potential models. In addition, the interfacial coordination number was also calculated, which varies depending on the alkalinity of Li, Na, and K. Using the interfacial coordination number, the bond strength-coordination number was estimated, and found that the interfacial energy trend Li > Na > K is related to the bond strength-coordination number.

Key words

glass-crystal interfacial energy / molecular dynamics simulation / interatomic potentials / interfacial coordination number

引用本文

Chandra Saha LETON, Murata TETSUYA, Nakane SHINGO. 化学计量碱金属二硅酸盐玻璃-晶体界面能的分子动力学研究：基于晶体最小能量切割法. 硅酸盐学报, 2025 , 54 (4) : 1291 -1298 . DOI: 10.14062/j.issn.0454-5648.20250430

Chandra Saha LETON, Murata TETSUYA, Nakane SHINGO. Molecular Dynamics Studies of Interfacial Energy in Stochiometric Alkali Disilicate Glass-Crystals Based on Crystal Minimum Energy Cutting[J]. Journal of the Chinese Ceramic Society, 2025 , 54 (4) : 1291 -1298 . DOI: 10.14062/j.issn.0454-5648.20250430

参考文献

收起

2025年第54卷第4期

PDF下载

引用本文

BibTeX

文章信息

doi: 10.14062/j.issn.0454-5648.20250430

接收时间：2025-06-03
首发时间：2026-05-20
出版时间：2025-11-10

补充材料

相关文章

文章信息

作者

出版历史

收稿日期：2025-06-03
修回日期：2025-07-18

基金

作者信息

日本电气硝子株式会社基础技术事业部，滋贺县大津市 520-8639，日本

参考文献

分享链接

https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20250430

分享至

全文二维码

扫描看全文

引用本文

BibTeX

本文的引用情况

2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

关闭全屏

BibTeX
EndNote
RefWorks
TxT