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Article(id=1319726347203760188, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726331013742638, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250292, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1744732800000, receivedDateStr=2025-04-16, revisedDate=1746720000000, revisedDateStr=2025-05-09, acceptedDate=null, acceptedDateStr=null, onlineDate=1792576880502, onlineDateStr=2026-10-21, pubDate=1760889600000, pubDateStr=2025-10-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792576880502, onlineIssueDateStr=2026-10-21, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792576880502, creator=13701087609, updateTime=1792576880502, updator=13701087609, issue=Issue{id=1319726331013742638, tenantId=1146029695717560320, journalId=1263187385517883426, year='2025', volume='53', issue='10', pageStart='2753', pageEnd='3078', issueExtLink='null', onlineDate='null', pubDate='1760889600000', pubDateStr='2025-10-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792576876643, creator='13701087609', updateTime=1792577470184, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319728820630962433, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726331013742638, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319728820635156738, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726331013742638, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=2791, endPage=2798, ext={EN=ArticleExt(id=1319726347803545661, articleId=1319726347203760188, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Quantitative Prediction of Structure and Properties of Nd3+-Doped Phosphate Laser Glass, columnId=1321945025580216350, journalTitle=Journal of the Chinese Ceramic Society, columnName=Special Issue on Technological Progress and Industrial Development of Advanced Glass Materials—Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction

Nd3+-doped phosphate glasses, utilizing the 4F3/2 → 4I11/2 energy-level transition of Nd3+ ions, achieve 1.06 μm luminescence and have critical applications in optical communications, biomedical engineering, and defense technologies. However, the development of laser glasses depends on empirical trial-and-error approaches, requiring extensive experimentation to generate limited data. This paradigm suffers from inefficiency, prolonged cycles, high costs, and a lack of theoretical guidance. Moreover, the luminescent properties of rare-earth-doped glasses are closely tied to the local structure of the rare-earth ions. The intricate relationship between structure and performance renders most computational models for glass properties ineffective, severely hindering the rapid advancement of laser glasses. It is thus necessary to develop cross-scale computational methods that combine physical interpretability and extrapolation capabilities to enable accurate prediction and inverse design of luminescent properties for broad-composition Nd3+-doped phosphate glasses.

In this study, Nd3+-doped Li2O-MgO-Al2O3-P2O5 glasses were prepared. The local microstructure of Nd3+ in the glass as a statistical ensemble of its local environments in neighboring glassy compounds (NGCs) was described. Based on this theoretical framework, an NGCs model was proposed to quantitatively predict the luminescent properties of Nd3+-doped phosphate laser glasses, positing that the glass's luminescent properties could be equal to the statistical average of the corresponding properties of its NGCs. This work could provide a theoretical foundation for quantitatively calculating the local structure and luminescent properties of rare-earth-doped laser glasses.

Methods

In rare-earth-doped laser glasses, the luminescent properties were determined via the analysis of the local structure of the rare-earth ions. The local structure of rare-earth ions in multicomponent laser glasses as a statistical ensemble of their configurations in NGCs was simulated based on the broken ergodicity theory. The NGCs in the compositional space (i.e., Li2O·Al2O3·4P2O5, 9Li2O·3Al2O3·8P2O5, P2O5, Li2O·P2O5, Al2O3·3P2O5, Li2O·2MgO·P2O5, MgO·P2O5, Li2O·6MgO·3P2O5, Al2O3·P2O5, MgO·2P2O5 and 2MgO·Al2O3·P2O5) were identified via querying the Materials Project database for the quaternary phosphate system (i.e., Li2O-MgO-Al2O3-P2O5). The local microstructure and luminescent properties of all glass compositions in this system were derived from these 11 NGCs by the NGCs model.

The molecular dynamics (MD) simulations were performed by the Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS). The Morse potential, suitable for modeling short-range interactions in rare-earth-doped glasses, was employed. The long-range interactions were treated by the Ewald summation method (cutoff radius: 12.0 Å), while the short-range interactions were truncated at 8.0 Å. The glass quenching process was simulated at a fixed timestep of 2 fs. The initial structure was thermalized at 5000 K for 1.0 ns to eliminate memory effects. The system was then cooled to 3000 K in the canonical (NVT) ensemble at 5 K/ps. To simulate the experimental conditions, the system was equilibrated in the isothermal-isobaric (NPT) ensemble at 3000 K for 1.0 ns, allowing simultaneous relaxation of the simulation box dimensions and atomic positions. The further cooling to 300 K was conducted in the NPT ensemble at 0.5 K/ps, with intermediate equilibration steps at 2500, 2000, 1500, 1000 K, and 300 K (1 ns each), respectively. Finally, a 1 ns equilibration in the microcanonical (NVE) ensemble was performed, with atomic coordinates recorded every 5000 steps during the last 500 ps.

Results and Discussion

The radial distribution function g(r) and structure factor S(q), representing short- and medium-range structural orders, were calculated by both the NGCs model and MD simulations. The results from these methods have remarkable consistency, indicating the NGCs model's capability to quantitatively determine the local structural features of Nd3+ in Li2O-MgO-Al2O3-P2O5 glasses. Since the luminescent properties of rare-earth-doped glasses are governed by the local coordination environment, this agreement validates the NGCs model for predicting luminescent performance.

The NGCs model is further applied to calculate key luminescent properties, i.e., the emission cross-section (σe) and fluorescence lifetime (τ) of the 4F3/2→4I11/2 transition. The σe values increase monotonically with Li2O content, showing a maximum relative deviation of 1.72% from experimental data. For τ that is influenced by non-structural factors such as hydroxyl quenching and Nd3+ clustering, the maximum relative error is 6.19%. These results underscore the model's accuracy in predicting luminescent properties. A robust composition-property mapping is established via leveraging this model, enabling efficient screening of high-performance Nd3+-doped phosphate glass compositions.

A comprehensive analysis of 11,355 valid glass compositions within the glass-forming region reveals an inverse correlation between σe and τ, i.e., compositions with a higher σe typically exhibit a shorter τ. However, the model identifies a subset of optimized compositions with both high σe and extended τ, corresponding to Al2O3 (0-7%), MgO (10%-18%), and Li2O (1%-7%).

Conclusions

This study applied the NGCs model to analyze the local structure and luminescent properties of Nd3+-doped Li2O-MgO-Al2O3-P2O5 glasses. The calculated gRe (r) and SRe(q), reflecting short- and medium-range orders, aligned closely with the MD simulation results, indicating the model's precision in characterizing Nd3+ local structures. The model achieved exceptional accuracy in predicting luminescent properties, with maximum relative errors of 1.72% for σe and 6.19% for τ, compared to the experimental data. The systematic screening of the glass-forming region identified optimal compositional ranges (i.e., Al2O3: 0-7%, MgO: 10%-18%, Li2O: 1%-7%) that could simultaneously maximize σe and τ.

The NGCs model could provide a groundbreaking approach for designing advanced Nd3+-doped phosphate laser glasses via establishing a quantitative link between atomic-scale structures and macroscopic performance. This methodology could accelerate material discovery and reduce reliance on costly experimental iterations, paving an efficient way for the development of next-generation laser materials.

, authors=Yihong SHEN, Minbo WU, Zhenjie LUN, Di ZUO, Dongdan CHEN, Qi QIAN, Guoping DONG, Zhongmin YANG, authorsList=Yihong SHEN, Minbo WU, Zhenjie LUN, Di ZUO, Dongdan CHEN, Qi QIAN, Guoping DONG, Zhongmin YANG, authorCompany=null, correspAuthors=Minbo WU, Dongdan CHEN, authorNote=

SHEN Yihong (2000-), male, Master candidate. E-mail:

, correspAuthorsNote=
WU Minbo (1995-), male, Ph.D., Assistant Professor. E-mail: ;
CHEN Dongdan (1976-), female, Ph.D., Associate Professor.
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Nd3+掺杂磷酸盐玻璃因其较大的受激发射截面、高效能量转换效率以及高能量存储密度，在激光武器、光通信和生物医疗等前沿领域具有重要的应用前景。然而，稀土离子掺杂激光玻璃的研发主要依赖经验引导、简单循环的“试错法”模式，存在研发效率低、周期长、成本高等问题，严重阻碍了激光玻璃材料及器件的发展。以Nd3+掺杂Li2O-MgO-Al2O3-P2O5玻璃为研究对象，利用玻璃组分空间中的邻近玻璃态化合物（NGCs）来预测玻璃的Nd3+局域结构特征和发光性能。研究表明，在该玻璃体系中，通过NGCs预测的Nd3+局域结构特征参数与分子动力学模拟结果高度一致；在发光性能方面，通过NGCs预测的荧光寿命和受激发射截面值与实验值的最大相对误差仅分别为6.19%和1.72%。基于此方法，成功筛选出了荧光寿命长、受激发射截面高的Nd3+掺杂磷酸盐激光玻璃组分。该研究为新型激光玻璃的组分设计提供了一条快速、低成本、高效的新方法。

, authors=沈毅鸿, 吴敏波, 伦振杰, 左笛, 陈东丹, 钱奇, 董国平, 杨中民, authorsList=沈毅鸿, 吴敏波, 伦振杰, 左笛, 陈东丹, 钱奇, 董国平, 杨中民, authorCompany=null, correspAuthors=吴敏波, 陈东丹, authorNote=

沈毅鸿（2000—），男，硕士研究生。

, correspAuthorsNote=
吴敏波（1995—），男，博士，助理研究员。
陈东丹（1976—），女，博士，副教授。
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Nd3+掺杂磷酸盐激光玻璃结构与性能的定量预测
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沈毅鸿 , 吴敏波 , 伦振杰 , 左笛 , 陈东丹 , 钱奇 , 董国平 , 杨中民
硅酸盐学报 | 先进玻璃材料技术与产业发展专题—研究论文 2025,53(10): 2791-2798
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硅酸盐学报 |先进玻璃材料技术与产业发展专题—研究论文 2025 , 53 (10) : 2791 -2798
Nd3+掺杂磷酸盐激光玻璃结构与性能的定量预测
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沈毅鸿 , 吴敏波 , 伦振杰, 左笛, 陈东丹 , 钱奇, 董国平, 杨中民
作者信息
  • 华南理工大学材料科学与工程学院，华南理工大学物理与光电学院，发光材料与器件国家重点实验室，广东省光纤激光材料与应用技术重点实验室，广东省特种光纤材料与器件工程技术研究开发中心，广州 510000
通讯作者:
吴敏波（1995—），男，博士，助理研究员。
陈东丹（1976—），女，博士，副教授。
作者简介:

沈毅鸿（2000—），男，硕士研究生。

Quantitative Prediction of Structure and Properties of Nd3+-Doped Phosphate Laser Glass
Yihong SHEN , Minbo WU , Zhenjie LUN, Di ZUO, Dongdan CHEN , Qi QIAN, Guoping DONG, Zhongmin YANG
Affiliations
  • School of Materials Science and Engineering, School of Physics and Optoelectronics, The State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Fiber Laser Materials and Applied Techniques, Guangdong Engineering Technology Research and Development Center of Special Optical Fiber Materials and Devices, South China University of Technology, Guangzhou 510000, China
    • Corresponding Author:
    WU Minbo (1995-), male, Ph.D., Assistant Professor. E-mail: ;
    CHEN Dongdan (1976-), female, Ph.D., Associate Professor.

    SHEN Yihong (2000-), male, Master candidate. E-mail:

出版时间: 2025-10-20 doi: 10.14062/j.issn.0454-5648.20250292
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摘要
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Nd3+掺杂磷酸盐玻璃因其较大的受激发射截面、高效能量转换效率以及高能量存储密度，在激光武器、光通信和生物医疗等前沿领域具有重要的应用前景。然而，稀土离子掺杂激光玻璃的研发主要依赖经验引导、简单循环的“试错法”模式，存在研发效率低、周期长、成本高等问题，严重阻碍了激光玻璃材料及器件的发展。以Nd3+掺杂Li2O-MgO-Al2O3-P2O5玻璃为研究对象，利用玻璃组分空间中的邻近玻璃态化合物（NGCs）来预测玻璃的Nd3+局域结构特征和发光性能。研究表明，在该玻璃体系中，通过NGCs预测的Nd3+局域结构特征参数与分子动力学模拟结果高度一致；在发光性能方面，通过NGCs预测的荧光寿命和受激发射截面值与实验值的最大相对误差仅分别为6.19%和1.72%。基于此方法，成功筛选出了荧光寿命长、受激发射截面高的Nd3+掺杂磷酸盐激光玻璃组分。该研究为新型激光玻璃的组分设计提供了一条快速、低成本、高效的新方法。

激光玻璃  /  磷酸盐玻璃  /  钕离子  /  邻近玻璃态化合物  /  定量预测
Introduction

Nd3+-doped phosphate glasses, utilizing the 4F3/2 → 4I11/2 energy-level transition of Nd3+ ions, achieve 1.06 μm luminescence and have critical applications in optical communications, biomedical engineering, and defense technologies. However, the development of laser glasses depends on empirical trial-and-error approaches, requiring extensive experimentation to generate limited data. This paradigm suffers from inefficiency, prolonged cycles, high costs, and a lack of theoretical guidance. Moreover, the luminescent properties of rare-earth-doped glasses are closely tied to the local structure of the rare-earth ions. The intricate relationship between structure and performance renders most computational models for glass properties ineffective, severely hindering the rapid advancement of laser glasses. It is thus necessary to develop cross-scale computational methods that combine physical interpretability and extrapolation capabilities to enable accurate prediction and inverse design of luminescent properties for broad-composition Nd3+-doped phosphate glasses.

In this study, Nd3+-doped Li2O-MgO-Al2O3-P2O5 glasses were prepared. The local microstructure of Nd3+ in the glass as a statistical ensemble of its local environments in neighboring glassy compounds (NGCs) was described. Based on this theoretical framework, an NGCs model was proposed to quantitatively predict the luminescent properties of Nd3+-doped phosphate laser glasses, positing that the glass's luminescent properties could be equal to the statistical average of the corresponding properties of its NGCs. This work could provide a theoretical foundation for quantitatively calculating the local structure and luminescent properties of rare-earth-doped laser glasses.

Methods

In rare-earth-doped laser glasses, the luminescent properties were determined via the analysis of the local structure of the rare-earth ions. The local structure of rare-earth ions in multicomponent laser glasses as a statistical ensemble of their configurations in NGCs was simulated based on the broken ergodicity theory. The NGCs in the compositional space (i.e., Li2O·Al2O3·4P2O5, 9Li2O·3Al2O3·8P2O5, P2O5, Li2O·P2O5, Al2O3·3P2O5, Li2O·2MgO·P2O5, MgO·P2O5, Li2O·6MgO·3P2O5, Al2O3·P2O5, MgO·2P2O5 and 2MgO·Al2O3·P2O5) were identified via querying the Materials Project database for the quaternary phosphate system (i.e., Li2O-MgO-Al2O3-P2O5). The local microstructure and luminescent properties of all glass compositions in this system were derived from these 11 NGCs by the NGCs model.

The molecular dynamics (MD) simulations were performed by the Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS). The Morse potential, suitable for modeling short-range interactions in rare-earth-doped glasses, was employed. The long-range interactions were treated by the Ewald summation method (cutoff radius: 12.0 Å), while the short-range interactions were truncated at 8.0 Å. The glass quenching process was simulated at a fixed timestep of 2 fs. The initial structure was thermalized at 5000 K for 1.0 ns to eliminate memory effects. The system was then cooled to 3000 K in the canonical (NVT) ensemble at 5 K/ps. To simulate the experimental conditions, the system was equilibrated in the isothermal-isobaric (NPT) ensemble at 3000 K for 1.0 ns, allowing simultaneous relaxation of the simulation box dimensions and atomic positions. The further cooling to 300 K was conducted in the NPT ensemble at 0.5 K/ps, with intermediate equilibration steps at 2500, 2000, 1500, 1000 K, and 300 K (1 ns each), respectively. Finally, a 1 ns equilibration in the microcanonical (NVE) ensemble was performed, with atomic coordinates recorded every 5000 steps during the last 500 ps.

Results and Discussion

The radial distribution function g(r) and structure factor S(q), representing short- and medium-range structural orders, were calculated by both the NGCs model and MD simulations. The results from these methods have remarkable consistency, indicating the NGCs model's capability to quantitatively determine the local structural features of Nd3+ in Li2O-MgO-Al2O3-P2O5 glasses. Since the luminescent properties of rare-earth-doped glasses are governed by the local coordination environment, this agreement validates the NGCs model for predicting luminescent performance.

The NGCs model is further applied to calculate key luminescent properties, i.e., the emission cross-section (σe) and fluorescence lifetime (τ) of the 4F3/2→4I11/2 transition. The σe values increase monotonically with Li2O content, showing a maximum relative deviation of 1.72% from experimental data. For τ that is influenced by non-structural factors such as hydroxyl quenching and Nd3+ clustering, the maximum relative error is 6.19%. These results underscore the model's accuracy in predicting luminescent properties. A robust composition-property mapping is established via leveraging this model, enabling efficient screening of high-performance Nd3+-doped phosphate glass compositions.

A comprehensive analysis of 11,355 valid glass compositions within the glass-forming region reveals an inverse correlation between σe and τ, i.e., compositions with a higher σe typically exhibit a shorter τ. However, the model identifies a subset of optimized compositions with both high σe and extended τ, corresponding to Al2O3 (0-7%), MgO (10%-18%), and Li2O (1%-7%).

Conclusions

This study applied the NGCs model to analyze the local structure and luminescent properties of Nd3+-doped Li2O-MgO-Al2O3-P2O5 glasses. The calculated gRe (r) and SRe(q), reflecting short- and medium-range orders, aligned closely with the MD simulation results, indicating the model's precision in characterizing Nd3+ local structures. The model achieved exceptional accuracy in predicting luminescent properties, with maximum relative errors of 1.72% for σe and 6.19% for τ, compared to the experimental data. The systematic screening of the glass-forming region identified optimal compositional ranges (i.e., Al2O3: 0-7%, MgO: 10%-18%, Li2O: 1%-7%) that could simultaneously maximize σe and τ.

The NGCs model could provide a groundbreaking approach for designing advanced Nd3+-doped phosphate laser glasses via establishing a quantitative link between atomic-scale structures and macroscopic performance. This methodology could accelerate material discovery and reduce reliance on costly experimental iterations, paving an efficient way for the development of next-generation laser materials.

laser glass  /  phosphate glass  /  neodymiumion  /  neighboring glassy compounds  /  quantitative prediction
沈毅鸿, 吴敏波, 伦振杰, 左笛, 陈东丹, 钱奇, 董国平, 杨中民. Nd3+掺杂磷酸盐激光玻璃结构与性能的定量预测. 硅酸盐学报, 2025 , 53 (10) : 2791 -2798 . DOI: 10.14062/j.issn.0454-5648.20250292
Yihong SHEN, Minbo WU, Zhenjie LUN, Di ZUO, Dongdan CHEN, Qi QIAN, Guoping DONG, Zhongmin YANG. Quantitative Prediction of Structure and Properties of Nd3+-Doped Phosphate Laser Glass[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (10) : 2791 -2798 . DOI: 10.14062/j.issn.0454-5648.20250292
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  • 国家自然科学基金(62235014)
  • 博士后自然科学基金面上项目(2024M760950)
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doi: 10.14062/j.issn.0454-5648.20250292
  • 接收时间：2025-04-16
  • 首发时间：2026-10-21
  • 出版时间：2025-10-20
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  • 收稿日期：2025-04-16
  • 修回日期：2025-05-09
基金
国家自然科学基金(62235014)
博士后自然科学基金面上项目(2024M760950)
作者信息
    华南理工大学材料科学与工程学院，华南理工大学物理与光电学院，发光材料与器件国家重点实验室，广东省光纤激光材料与应用技术重点实验室，广东省特种光纤材料与器件工程技术研究开发中心，广州 510000

通讯作者:

吴敏波（1995—），男，博士，助理研究员。
陈东丹（1976—），女，博士，副教授。
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