物理学报2017，Vol.66Issue(11)：243-250,8.DOI:10.7498/aps.66.116501
聚乙烯单链量子热输运的同位素效应
Isotope effect on quantum thermal transport in a polyethylene chain
摘要
Abstract
Effective control of thermal conductive property of polymeric materials is now attracting more and more attention from both the theoretical and the experimental aspects.Bulk polyethylene is regarded as a thermal insulator because its thermal conductivity is typically on the order of 0.35 W.m-1.K-1.However,recent studies demonstrate that a polyethylene chain has an extremely high thermal conductivity and the reported thermal conductivity of ultra-drawn polyethylene nanofibers is as high as 104 W·m-1·K-1,about 300 times higher than that of bulk polyethylene.In order to cast off this dilemma,several simulation methods are used to detect the unusually high thermal conductivity of a polyethylene chain.Molecular dynamics (MD) simulation results are highly sensitive to the choice of empirical potential or simulation method.Even using the same potential (AIREBO potential),the obtained thermal conductivity of a polyethylene chain is different.By combining the Green-Kubo method with a modal decomposition approach,equilibrium molecular dynamics (EMD) indicates that the thermal conductivity is able to exceed 100 W.m-LK-1 whilethe polyethylene chain is longer than 40 nm at room temperature.Compared with the simulation result obtained by equilibrium molecular dynamics,the simulation result provided by using the non-equilibrium molecular dynamics (NEMD) method is only 57 W.m-1.K-1 for a 160-nm-long polyethylene chain at room temperature.We use the first-principles method to calculate the force constant tensor,and the characteristics of quantum thermal transport in a polyethylene chain can be revealed.In our algorithm,several shortcomings of molecular dynamics,i.e.,different potential functions or simulation methods may lead to obviously different results for the same quantum thermal transport system,are overcome.Based on the density functional theory (DFT),the central insertion scheme (CIS) combined with nonequilibrium Green's function (NEGF) is used to evaluate the isotope effect on quantum thermal transport in a polyethylene chain,which includes 432 atoms in scattering region and has a length of 18.533 nm.It is found that the upper limit of thermal conductivity of a 100-nm-long pure12C polyethylene chain reaches a high value of 314.1 W.m LK-1 at room temperature.Moreover,for the case of a pure polyethylene chain of 12C,with other conditions unchanged,the reduction of average thermal conductance caused by 14C impurity is more remarkable than that by 13C.The most outstanding isotope effect on quantum thermal transport can be detected in the polyethylene chain.When the doping concentration of 14C in 12C is 50％ at room temperature,the average thermal conductance will be reduced by 51％.It is of great significance for studying the mechanism of isotope effect on thermal transport in polyethylene.关键词
聚乙烯单链/量子热输运/平均热导/同位素效应Key words
polyethylene chains/quantum thermal transport/average thermal conductance/isotope effect引用本文复制引用
吴宇,蔡绍洪,邓明森,孙光宇,刘文江,岑超..聚乙烯单链量子热输运的同位素效应[J].物理学报,2017,66(11):243-250,8.基金项目
Project supported by the National Natural Science Foundation of China (Grant No.11264005),the Foundation of Science and Technology of Guizhou Province,China (Grant No.J[2012]2292),and the Natural Science Foundation of the Education Department of Guizhou Province,China (Grant Nos.[2014]307,2008057,2007036).国家自然科学基金(批准号:11264005)、贵州省科学技术基金(批准号:黔科合J字[2012]2292号)、贵州省教育厅自然科学研究项目(批准号:黔教合KY字[2014]307,黔教科2008057,2007036)资助的课题. （Grant No.11264005）
