SrTiO3材料中氧空位的密度泛函理论

Oxygen vacancies in SrTiO3 by density function theory

  • 摘要: 计算了SrTiO3-δ(δ=0,δ=0.125)体系电子结构,分析了氧空位对SrTiO3晶体的价键结构、能带、态密度、分波态密度、差分电荷密度的影响。所有计算都是基于密度泛函理论(DFT)框架下的第一性原理平面波超软赝势方法。计算结果表明:当氧空位浓度δ=0.125时,空位在母体化合物SrTiO3中引入了大量的传导电子,费米能级进入导带,体系显示金属型导电性。由于空位掺杂,导带底附近的态密度发生了畸变,刚性能带模型不再适合描述SrTiO2.875体系。同时,在导带底附近距离费米能级0.3eV处引入了空位能级,这和实验测得的SrTiO3材料内中性氧空位的电离能约为0.4eV相符。此外,Mulliken布局分析、分波态密度和差分电荷密度分析表明,该空位能级主要由与其最近邻的两个Ti原子的3d电子态贡献,并且由该空位引入的导电电子大部分都局域在空位最近邻的两个Ti原子周围。最后,计算了三种典型平衡条件下SrTiO3晶体内中性氧空位的形成能。

     

    Abstract: The electronic structure calculations including the Mulliken population analysis,band structure,density of states(DOS),partial density of states(PDOS)and electron density difference on SrTiO3-δwithδ=0 andδ=0.125 were performed by the first-principles calculation of plane wave ultrasoft pseudo-potential technology based on the density function theory(DFT).The calculated results revealed that due to the oxygen(O)vacancy electron doping,the Fermi level moved into conduction bands (CBs)for SrTiO3-δwithδ=0.125 and the system showed metallic behavior.There was a new defect level below the bottommost of CBs when one O vacancy was introduced.The 3d states of the two Ti atoms nearest to the vacancy made significant contribution to it.The electrons introduced by the O vacancy were largely localized on the two nearest Ti atoms.Furthermore,the formation energies of neutral O vacancy were calculated in three typical equilibrium conditions.

     

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