近十年中国同位素效应理论和计算研究进展  

Ten-year Progresses in Computational and Theoretical Isotope Effect Studies in China

作　　者：刘耘[1,2,3] LIU Yun(State Key Laboratory of Ore Deposit Geochemistry,Institute of Geochemistry,Chinese Academy of Sciences,Guiyang 550081,China;International Research Center for Planetary Science,College of Earth Sciences,Chengdu University of Technology,Chengdu 610059,China;CAS Center for Excellence in Comparative Planetology y Hefei 230026,China)

机构地区：[1]矿床地球化学国家重点实验室,中国科学院地球化学研究所,贵阳550081 [2]成都理工大学行星科学国际研究中心,成都610059 [3]中国科学院比较行星学卓越创新中心,合肥230026

出　　处：《矿物岩石地球化学通报》2021年第6期1287-1303,共17页Bulletin of Mineralogy, Petrology and Geochemistry

基　　金：中国科学院先导专项B子课题(XDB41000000);中国航空航天局民用技术项目(CNSA-D020202)。

摘　　要：近十年来,国内稳定同位素地球化学的理论解释已普遍达到了量子化学水平。基于精密的量子化学从头或第一性原理,研究者们开始了平衡和动力学分馏系数的计算。在同位素的分析测试、野外观察、理论和计算四个方向上,国内在理论和计算方向的发展可能还算最好的,整体处于国际第一方阵的地位。国内学者率先发展了超冷体系同位素分馏、含压力效应的同位素分馏、同位素的浓度效应、团簇同位素、微小同位素异常、热梯度下同位素扩散效应、高温重复过程等方向的同位素理论和计算方法,也发展了针对固-液两相同位素分馏的可变体积的分子簇(VVCM)计算新方法、针对重金属同位素固相体系的含核体积效应处理的方法,以及针对熔体中同位素扩散的动力学分馏的理论和计算方法。同时,还为大量不同的非传统(金属)同位素体系,提供了大量的平衡分馏系数,为这些同位素体系的日后深入应用奠定了较好的基础。但是,在这些成果中,真正由我国学者首先提出的原始概念、模型、体系和方法还很少,绝大多数都是对前人(主要是国外同行)提出的理论体系和新兴发展方向的修改和补充。未来我国同位素理论和计算领域应率先使用包含量子场论在内的新一代理论工具,在同位素效应的新方向、新概念的提出和新理论的建立方面,做出更多的贡献。During the past decade, the stable isotope geochemical theory for interpreting stable isotope fractionation has commonly reached the level of quantum chemistry in China. Based on the precise ab initio or first principles of quantum chemistry, researchers started to routinely undertake the equilibrium and kinetic isotope fractionation coefficient calculations. Among the four sub-fields of isotope geochemistry, i.e., laboratory analysis, field observation, computation, and theoretical studies, I am proud to say that computation and theoretical studies of isotope geochemistry in China have made important contributions over the past ten years, enjoying a status on par with the cutting-edge researches in the world. Chinese researchers have taken the lead in several new areas of the theoretical and calculation methods of isotope geochemistry, including isotope fractionations under super-cold conditions, isotope fractionation with pressure effects, concentration-dependent isotope effects, clumped isotope effects, small isotope anomaly, isotope diffusion effects under thermal gradient, and high temperature repeated-process isotope effects. They have also developed some new computational methods for stable isotope effects, including a variable volume cluster model(VVCM) method for computing equilibrium isotope fractionation between solid and liquid phases, methods considering nuclear-volume effect for heavy metal isotope in solid phase systems, and methods for the theoretical calculation of equilibrium and kinetic fractionations of the isotope diffusion in silicate melts. Meanwhile, they have provided a large number of needed equilibrium or kinetic isotope fractionation coefficients or parameters for a large number of various non-traditional or metal isotope systems which have broad applications in geological and planetary sciences. Their adventures have laid a good foundation for the future in-depth application of these isotope systems. However, Chinese researchers must recognize that most of the new concepts, models, sy

关 键 词：同位素效应 稳定同位素分馏 理论计算 量子化学 平衡分馏 超冷体系 压力效应 同位素浓度效应 

分 类 号：P597[天文地球—地球化学]