量子力学中的Roothaan-Hartree-Fock(R-H-F)近似计算在原子、分子和材料电子结构计算中具有重要的意义,是其他高精度电子结构计算方法的基础.本工作根据开源网站Basis Set Exchange中丰富的基组资源,利用高斯型基组矩阵元具有解析表达...量子力学中的Roothaan-Hartree-Fock(R-H-F)近似计算在原子、分子和材料电子结构计算中具有重要的意义,是其他高精度电子结构计算方法的基础.本工作根据开源网站Basis Set Exchange中丰富的基组资源,利用高斯型基组矩阵元具有解析表达式的特性,自行编写Roothaan-Hartree-Fock计算程序,可以较为方便的达到高精度的计算结果.同时本工作用不同大小的基组计算了多种原子和离子的基态能量,研究了He、Be、C2+等原子和离子在不同基组下的收敛特性.此外,基于自行编写的R-H-F程序计算得到He、Be、Ne的第一电离能,与实验对比最大误差不超过6.84%.展开更多
The discovery of ferroelectricity in HfO_(2)-based materials with high dielectric constant has inspired tremendous research interest for next-generation electronic devices.Importantly,films structure and strain are ke...The discovery of ferroelectricity in HfO_(2)-based materials with high dielectric constant has inspired tremendous research interest for next-generation electronic devices.Importantly,films structure and strain are key factors in exploration of ferroelectricity in fluorite-type oxide HfO_(2) films.Here we investigate the structures and straininduced ferroelectric transition in different phases of few-layer HfO_(2) films(layer number𝑁=1–5).It is found that HfO_(2) films for all phases are more stable with increasing films thickness.Among them,the Pmn2_(1)(110)-oriented film is most stable,and the films of𝑁=4,5 occur with a𝑃21 ferroelectric transition under tensile strain,resulting in polarization about 11.8μC/cm^(2) along in-plane𝑎-axis.The ferroelectric transition is caused by the strain,which induces the displacement of Hf and O atoms on the surface to non-centrosymmetric positions away from the original paraelectric positions,accompanied by the change of surface Hf–O bond lengths.More importantly,three new stable HfO_(2)2D structures are discovered,together with analyses of computed electronic structures,mechanical,and dielectric properties.This work provides guidance for theoretical and experimental study of the new structures and strain-tuned ferroelectricity in freestanding HfO_(2) films.展开更多
文摘量子力学中的Roothaan-Hartree-Fock(R-H-F)近似计算在原子、分子和材料电子结构计算中具有重要的意义,是其他高精度电子结构计算方法的基础.本工作根据开源网站Basis Set Exchange中丰富的基组资源,利用高斯型基组矩阵元具有解析表达式的特性,自行编写Roothaan-Hartree-Fock计算程序,可以较为方便的达到高精度的计算结果.同时本工作用不同大小的基组计算了多种原子和离子的基态能量,研究了He、Be、C2+等原子和离子在不同基组下的收敛特性.此外,基于自行编写的R-H-F程序计算得到He、Be、Ne的第一电离能,与实验对比最大误差不超过6.84%.
基金supported by the National Key R&D Program of China(Grant No.2023YFB4402600)the National Natural Science Foundation of China(Grant Nos.12074241,11929401,52130204,12311530675,and 52271007)+5 种基金Key Research Project of Zhejiang Lab(Grant No.2021PE0AC02)Science and Technology Commission of Shanghai Municipality(Grant Nos.22XD1400900,20501130600,21JC1402700,and 21JC1402600)supports from the open projects of Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials(Anhui University of Technology),Ministry of Education(Grant No.GFST2022KF08)State Key Laboratory of Surface Physics(Fudan University)(Grant No.KF202210)State Key Laboratory of Infrared Physics,Shanghai Institute of Technical Physics,Chinese Academy of Sciences(Grant No.SITP-NLIST-YB-2022-08)the support of China Scholarship Council,and thanks Mr.Xiaowen Shi(from HZWTECH)for helpful discussions.
文摘The discovery of ferroelectricity in HfO_(2)-based materials with high dielectric constant has inspired tremendous research interest for next-generation electronic devices.Importantly,films structure and strain are key factors in exploration of ferroelectricity in fluorite-type oxide HfO_(2) films.Here we investigate the structures and straininduced ferroelectric transition in different phases of few-layer HfO_(2) films(layer number𝑁=1–5).It is found that HfO_(2) films for all phases are more stable with increasing films thickness.Among them,the Pmn2_(1)(110)-oriented film is most stable,and the films of𝑁=4,5 occur with a𝑃21 ferroelectric transition under tensile strain,resulting in polarization about 11.8μC/cm^(2) along in-plane𝑎-axis.The ferroelectric transition is caused by the strain,which induces the displacement of Hf and O atoms on the surface to non-centrosymmetric positions away from the original paraelectric positions,accompanied by the change of surface Hf–O bond lengths.More importantly,three new stable HfO_(2)2D structures are discovered,together with analyses of computed electronic structures,mechanical,and dielectric properties.This work provides guidance for theoretical and experimental study of the new structures and strain-tuned ferroelectricity in freestanding HfO_(2) films.
