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Optimizing and extending ion dielectric polarizability database for microwave frequencies using machine learning methods
发布时间:2023-09-19

Optimizing and extending ion dielectric polarizability database for microwave frequencies using machine learning methods

    Jincheng Qin, Zhifu Liu, Mingsheng Ma & Yongxiang Li
 

    npj Computational Materials 9: 132 (2023)
   doi.org/10.1038/s41524-023-01093-6
    Published online: 28 July 2023
   AbstractFull Text | PDF OPEN
  

  
Abstract:  Permittivity at microwave frequencies determines the practical applications of microwave dielectric ceramics. The accuracy and universality of the permittivity prediction by Clausius-Mossotti equation depends on the dielectric polarizability ( D) database. The most influential D database put forward by Shannon is facing three challenges in the 5G era: (1) Few data, (2) Simplistic relation and (3) Low frequency (kHz ~ MHz) oriented. Here, we optimized and extended the Shannon’s database for microwave frequencies by the four-stage multiple linear regression and support vector machine model. In comparison with the conventional database, the optimized and extended databases achieved higher accuracy and expanded the amount of data from 60 to more than 900. Besides, we analyzed the relationships between D and ion characteristics, including ionic radius (IR), atomic number (N), valence state (V) and coordination number (CN). We found that the positive cubic law of “ D ~ IR3” discussed in Shannon’s work was valid for the IR changed by the N, but invalid for the change caused by the CN.
摘要:  微波频率下的介电常数决定了微波介质陶瓷的实际应用。Clausius-Mossotti方程预测介电常数的准确性和普适性取决于介电极化率( D)数据库。当今最具影响力的 D数据库由Shannon提出,然而在5G时代面临三大挑战:(1)数据量小、(2)规律过于简化、(3)面向低频(kHz ~ MHz)。本文面向微波频段采用四阶段多元线性回归和支持向量机模型对Shannon数据库进行了优化和扩展。与传统数据库相比,优化和扩展后的数据库准确性更高,且数据量从60个扩展至900余个。此外,我们还分析了 D与离子半径(IR)、原子序数(N)、价态(V)和配位数(CN)等离子特性之间的关系。我们发现Shannon工作中讨论的“ D ~ IR3”正三次方律对于由N引起的IR变化是成立的,但对于由CN引起的IR变化则失效。
Editorial Summary

Ion dielectric polarizability database: Optimizing and extending by machine learning

Permittivity determines the practical applications of microwave dielectric materials, so accurate prediction of permittivity is an important task of the materials design on demand. Both classical dielectric theory and recent machine learning studies indicate that the ion dielectric polarizability ( D) is the decisive parameter for permittivity prediction. However, the most influential D database, put forward by Shannon in 1993, is facing three challenges in the 5G era: (1) Few data, (2) Simplistic relation and (3) Low frequency (kHz ~ MHz) oriented. Therefore, it cannot satisfy the accurate permittivity prediction of novel microwave dielectric materials for GHz band applications. Machine learning methods enable quantitative, accurate, efficient and low-cost prediction of material properties, and also shows advantages in mining hidden physical relationship. Thus, it opens up a new path for optimizing and extending the D database.A team led by Prof. Zhifu Liu from Shanghai Institute of Ceramics, Chinese Academy of Sciences, optimized and extended the ion dielectric polarizability database by multiple linear regression and support vector machine methods, achieving improved accuracy of D data, and greatly expanding the data amount from 61 to 915, covering 92 elements.In this work, based on the permittivity data of 334 microwave dielectric ceramics reported in literatures, the current D data was optimized according to the error degree by four-stage multiple linear regression method. Based on the optimized database, several machine learning models were used to try to establish the quantitative relationship between the D value and basic characteristics of ion. The optimal model, based on support vector machine algorithm and including atomic number (N), valence state (V), coordination number (CN) and ion radius (IR), was used to extend the D database. Combining dielectric theory and SHAP method, this work discussed the mechanism of basic characteristics of ion affecting the D value, and also found that the neglected importance of V and CN on the D value in previous studies. The previously found positive linear relation between the D value and the cube of ionic radius is valid for the ions with the same V and CN, meaning the change of IR caused by N. However, the law fails when the change of IR caused by CN, for ions with the same V and N. In addition, the D databases were integrated and publicly available online (https://qincas.gitee.io/idp-ml/), which serves as a reference for the research and development of microwave dielectric materials.

离子介电极化率数据库:机器学习优化及拓展

介电常数决定电介质材料的实际应用,准确计算和预测介电常数是实现微波介质材料按需设计的重要一环。经典介电理论和最新机器学习研究均指出离子介电极化率( D)是预测介电常数的决定性参量。然而,当今最具影响力的、由Shannon于1993年给出的 D数据库在5G/6G时代面临着三大挑战:①数据量少、②离子基本属性对 D的影响考虑较少、③仅面向低频段(kHz ~ MHz),因此不能满足面向GHz频段应用的新型微波介质材料的介电常数准确计算和预测。机器学习方法在材料性能预测和挖掘数据背后隐含物理关系等问题中表现出定量、准确、高效、低成本等优势,这为 D数据库的优化及拓展开辟了新路径。中国科学院上海硅酸盐研究所的刘志甫研究员团队采用多元线性回归和支持向量机方法优化并拓展了离子介电极化率数据库,实现 D数据准确性的提升,同时将数据量从61种大幅扩充至915种,覆盖92种元素。该工作基于文献报道的334种微波介质陶瓷的介电常数数据,依据目前 D数据的误差程度,采用四阶段多元线性回归方法对不同 D数据进行优化。基于优化后的数据库,采用多种机器学习模型尝试建立 D值与离子基本属性之间的定量关系,并利用最优模型拓展 D数据库。模型寻优表明,最优模型基于支持向量机算法,包含原子序数(N)、价态(V)、配位数(CN)和离子半径(IR)四个特征量。该工作还结合电介质理论知识和归因分析SHAP方法,讨论了离子基本属性对 D值的作用机制,并发现前人的研究忽视了V和CN对 D值的重要影响,所总结的 D值与离子半径三次方之间的正线性关系并非总是成立:对于V和CN相同的离子,IR的变化由N引起,规律成立;但对于V和N相同的离子,IR的变化由CN引起,规律失效。基于该工作,作者还建立了一个在线 D数据库(https://qincas.gitee.io/idp-ml/),为微波介质材料领域的研究者提供参考。

 
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