基于多体摄动理论的CaO电子能带结构及光吸收谱的研究
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摘要
使用多体摄动理论研究了碱土金属氧化物CaO的电子激发态和光吸收谱.运用GW近似方法来改进DFT对电子交换关联的处理,并计算了CaO电子能带结构.考虑到电子与空穴的相互作用,运用二粒子格林函数理论来求解Bethe-Salpeter方程,计算电子-空穴激发态,并在此基础上计算光吸收谱.计算结果 CaO能隙为7.0 e V,与实验结果 7.1 e V符合很好;并且CaO光吸收谱的理论结果与实验数据也相符合.
This paper reports the electronic band structure and the optical absorption spectrum of alkaline-earth metal oxide Ca O, using many-body perturbation theory. The quasiparticle band structure is calculated within the GW approximation. By taking the electron-hole interaction into consideration, electron-hole pair states and optical excitations are obtained by solving the Bethe-Salpeter equation for the electron-hole two-particle Green function. The calculated band gap for Ca O is 7.0 e V, which is in good agreement with the experimental result of 7.1 e V. The theoretical results of optical absorption spectrum for Ca O are also in agreement with the experimental data.
This paper reports the electronic band structure and the optical absorption spectrum of alkaline-earth metal oxide Ca O, using many-body perturbation theory. The quasiparticle band structure is calculated within the GW approximation. By taking the electron-hole interaction into consideration, electron-hole pair states and optical excitations are obtained by solving the Bethe-Salpeter equation for the electron-hole two-particle Green function. The calculated band gap for Ca O is 7.0 e V, which is in good agreement with the experimental result of 7.1 e V. The theoretical results of optical absorption spectrum for Ca O are also in agreement with the experimental data.
引文
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[19]ROHLFING M,LOUIE S G.Document electron-hole excitations and optical spectra from first principles[J].Physical Review B,2000,62:4927-4944.
[20]MADELUNG O.Semiconductors:Data Handbook[M].3rd ed.Berlin:Springer,2004:62-68.
[21]WHITED R C,FLATEN C J,WALKER W C.Exciton thermoreflectance of Mg O and Ca O[J].Solid State Commun,1973,13:1903-1905.
[2]KOHN W,SHAM L J.Self-consistent equations including exchange and correlation effects[J].Physical Review A,1965,140:1133-1138.
[3]PEDEW J P,BURKE K,ERNZERHOF M.Generalized gradient approximation made simple[J].Phys Rev Lett,1996,77:3865-3868.
[4]OHNO K,ESFARJANI K,KAWAZOE Y.Computational Materials Science[M].Berlin:Springer Presses,1999:66-102.
[5]ONIDA L.REINING A R.Electronic excitations:Densityfunctional versus many-body Green’s-function approaches[J].Reviews of Modern Physics,2002,74:601-659.
[6]CHING W Y,GAN F,HUANG M Z.Band theory of linear and nonlinear susceptibilities of some binary ionic insulators[J].Physical Review B,1995,52:1596-1611.
[7]DADSETANI M,BEIRANVAND R.Optical properties of alkaline-earth metal oxides from first principle[J].Solid State Sciences,2009,11:2099-2105.
[8]KANEKO Y,MORIMOTO K,KODA T.Optical properties of alkaline-earth chalcogenides.II.Vacuum ultraviolet reflection spectra in the synchrotron radiation region of 4-40 e V[J].Journal of the Physical Society of Japan,1988,52:4385-4396.
[9]HANKE W,SHAM L J.Many-particle effects in the optical spectrum of a semiconductor[J].Physical Review B,1980,21:4656-4673.
[10]HEDIN L.New method for calculating the one-particle Green’s function with application to the electron-gas problem[J].Physical Review A,1965,139:796-823.
[11]HEDIN L,LUNDQVIST S.Effects of electron-electron and electron-phonon interactions on the one-electron states of solids[J].Solid State Physics,1970,23:1-181
[12]BACHELET G B,HAMANN D R,SCHLüTER M.Pseudopotentials that work:From H to Pu[J].Physical Review B,1982,26:4199-4228.
[13]ROHLFING M,KRüGER P,POLLMANN J.Efficient scheme for GW quasiparticle band-structure calculations with applications to bulk Si and to the Si(001)-(2×1)surface[J].Physical Review B,1995,52:1905-1917.
[14]ROHLFING M,KRüGER P,POLLMANN J.Quasiparticle band-structure calculations for C,Si,Ge,Ga As,and Si C using Gaussian-orbital basis sets[J].Physical Review B,1993,48:17791-17805.
[15]HYBERTSEN M S,LOUIE S G.Model dielectric matrices for quasiparticle self-energy calculations[J].Physical Review B,1988,37:2733-2736.
[16]HYBERTSEN M S,LOUIE S G.Electron correlation in semiconductors and insulators:Band gaps and quasiparticle energies[J].Physical Review B,1986,34:5390-5413.
[17]FETTER A,WALECKA J D.Quantum Theory of Many Particle Systems[M].New York:Mc Graw-Hill Presses,1973:86-112.
[18]STRINATI G.Dynamical shift and broadening of core excitons in semiconductors[J].Physical Review Letters,1982,49:1519-1522.
[19]ROHLFING M,LOUIE S G.Document electron-hole excitations and optical spectra from first principles[J].Physical Review B,2000,62:4927-4944.
[20]MADELUNG O.Semiconductors:Data Handbook[M].3rd ed.Berlin:Springer,2004:62-68.
[21]WHITED R C,FLATEN C J,WALKER W C.Exciton thermoreflectance of Mg O and Ca O[J].Solid State Commun,1973,13:1903-1905.