Structural and electronic properties of Pb_(n)Ag_(n)(n=2–12)clusters were investigated by density functional theory with generalized gradient approximation at BLYP level in DMol3 program package.The optimized bimetal...Structural and electronic properties of Pb_(n)Ag_(n)(n=2–12)clusters were investigated by density functional theory with generalized gradient approximation at BLYP level in DMol3 program package.The optimized bimetallic Pb_(n)Ag_(n)(n=2–12)clusters were viewed as the initial structures,then,those were calculated by ab initio molecular dynamics(AIMD)to search possible global minimum energy structures of Pb_(n)Ag_(n)clusters,finally,the ground state structures of Pb_(n)Ag_(n)(n=2–12)clusters were achieved.According to the structural evolution of lowest energy structures,Ag atoms prefer gather in the central sites while Pb atoms prefer external positions in Pb_(n)Ag_(n)(n=2–12)clusters,which is in excellent agreement with experimental results from literature and the application in metallurgy.The average binding energies,HOMO-LUMO gaps,vertical ionization potentials,vertical electron affinities,chemical hardnessη,HOMO orbits,LUMO orbits and density of states of Pb_(n)Ag_(n)(n=2–12)clusters were calculated.The results indicate that the values of HOMO-LUMO gaps,vertical ionization potentials,vertical electron affinities and chemical hardnessηshow obvious odd-even oscillations when n≤5,Pb_(n)Ag_(n)(n=2–12)clusters become less chemically stable and show insulator-to-metal transition with the variation of cluster size n,Pb_(n)Ag_(n)(n≥9)cluster are good candidates to study the properties of PbAg alloys.Those can be well explained by the density of states(DOS)distributions of Pb atoms and Ag atoms between–0.5 Ha and 0.25 Ha in Pb_(n)Ag_(n)(n=2–12)clusters.展开更多
构建了系列球形中空结构的纳米线(NW),采用分子动力学(MD)对每个模型300个不同初始态的样本开展拉伸形变模拟。并利用基于密度的噪声应用空间聚类(density-based spatial clustering of applications with noise,DBSCAN)机器学习算法,...构建了系列球形中空结构的纳米线(NW),采用分子动力学(MD)对每个模型300个不同初始态的样本开展拉伸形变模拟。并利用基于密度的噪声应用空间聚类(density-based spatial clustering of applications with noise,DBSCAN)机器学习算法,获得了初始滑移面的位置。基于大数据统计,分析了初始滑移位置分布以及断裂位置分布两者之间的相关性。研究结果表明:当内部中空半径较小时,断裂位置分布形成于塑性形变阶段,初始滑移分布与断裂位置分布之间无显著的相关性;但是对于脆性特征明显的大中空半径的NW,高能内表面诱导产生的滑移面迅速积累,产生颈缩并导致最终的断裂。因此当内部中空结构达到一定尺寸时初始滑移位置的分布与最终断裂位置的分布之间有明确的因果关系。展开更多
基金Project(51664032)supported by the Regional Foundation of the National Natural Science Foundation of ChinaProject(51474116)supported by the General Program of the National Natural Science Foundation of China+5 种基金Project(U1502271)supported by the Joint Foundation of the NSFC-Yunnan Province,ChinaProject(2014HA003)supported by the Cultivating Plan Program for the Leader in Science and Technology of Yunnan Province,ChinaProject(2014RA4018)supported by the Program for Nonferrous Metals Vacuum Metallurgy Innovation Team of Ministry of Science and Technology,ChinaProject(2016YFC0400404)supported by the National Key Research and Development Program of ChinaProject(51504115)supported by the Youth Program of National Natural Science Foundation of ChinaProject(IRT_17R48)supported by the Program for Innovative Research Team in University of Ministry of Education of China
文摘Structural and electronic properties of Pb_(n)Ag_(n)(n=2–12)clusters were investigated by density functional theory with generalized gradient approximation at BLYP level in DMol3 program package.The optimized bimetallic Pb_(n)Ag_(n)(n=2–12)clusters were viewed as the initial structures,then,those were calculated by ab initio molecular dynamics(AIMD)to search possible global minimum energy structures of Pb_(n)Ag_(n)clusters,finally,the ground state structures of Pb_(n)Ag_(n)(n=2–12)clusters were achieved.According to the structural evolution of lowest energy structures,Ag atoms prefer gather in the central sites while Pb atoms prefer external positions in Pb_(n)Ag_(n)(n=2–12)clusters,which is in excellent agreement with experimental results from literature and the application in metallurgy.The average binding energies,HOMO-LUMO gaps,vertical ionization potentials,vertical electron affinities,chemical hardnessη,HOMO orbits,LUMO orbits and density of states of Pb_(n)Ag_(n)(n=2–12)clusters were calculated.The results indicate that the values of HOMO-LUMO gaps,vertical ionization potentials,vertical electron affinities and chemical hardnessηshow obvious odd-even oscillations when n≤5,Pb_(n)Ag_(n)(n=2–12)clusters become less chemically stable and show insulator-to-metal transition with the variation of cluster size n,Pb_(n)Ag_(n)(n≥9)cluster are good candidates to study the properties of PbAg alloys.Those can be well explained by the density of states(DOS)distributions of Pb atoms and Ag atoms between–0.5 Ha and 0.25 Ha in Pb_(n)Ag_(n)(n=2–12)clusters.
文摘构建了系列球形中空结构的纳米线(NW),采用分子动力学(MD)对每个模型300个不同初始态的样本开展拉伸形变模拟。并利用基于密度的噪声应用空间聚类(density-based spatial clustering of applications with noise,DBSCAN)机器学习算法,获得了初始滑移面的位置。基于大数据统计,分析了初始滑移位置分布以及断裂位置分布两者之间的相关性。研究结果表明:当内部中空半径较小时,断裂位置分布形成于塑性形变阶段,初始滑移分布与断裂位置分布之间无显著的相关性;但是对于脆性特征明显的大中空半径的NW,高能内表面诱导产生的滑移面迅速积累,产生颈缩并导致最终的断裂。因此当内部中空结构达到一定尺寸时初始滑移位置的分布与最终断裂位置的分布之间有明确的因果关系。