Nonlinear optics from an ab initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors
Nonlinear optics from an ab initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors
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DOI：
10.1103/physrevb.88.235113
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发表时间：
2013-09
影响因子：
3.7
通讯作者：
C. Attaccalite;M. Gruning
中科院分区：
文献类型：
--
作者：
C. Attaccalite;M. Gruning
我们提出了一个从头算的实时计算方法来研究凝聚态系统中的非线性光学性质，特别适合于结晶固体和周期性纳米结构。运动方程和电子与外部电场的耦合从动态极化的Berry相位公式导出[Souza等人，Phys. Rev. B 69，085106（2004）]。通过在独立粒子哈密顿量中加入单粒子算符引入多体效应。我们添加了一个Hartree算子来解释晶体的局部效应，并添加了一个Hartree算子来校正准粒子效应的独立粒子能带结构。我们还讨论了通过增加一个屏蔽的Hartree-Fock自能算子来精确处理激子效应的可能性。该方法通过计算SiC和AlAs块状半导体的二次谐波产生来验证：与频域中响应理论的现有从头计算获得了极好的一致性[Luppi等人，Phys. Rev. B 82，235201（2010）]。最后，我们展示的应用程序的二次谐波产生的碲化镉和三次谐波产生的硅。
We present an ab-initio real-time-based computational approach to study nonlinear optical properties in condensed matter systems that is especially suitable for crystalline solids and periodic nanostructures. The equations of motion and the coupling of the electrons with the external electric field are derived from the Berry-phase formulation of the dynamical polarization [Souza et al., Phys. Rev. B 69, 085106 (2004)]. Many-body effects are introduced by adding single-particle operators to the independent-particle Hamiltonian. We add a Hartree operator to account for crystal local effects and a scissor operator to correct the independent particle band structure for quasiparticle effects. We also discuss the possibility of accurately treating excitonic effects by adding a screened Hartree-Fock self-energy operator. The approach is validated by calculating the second-harmonic generation of SiC and AlAs bulk semiconductors: an excellent agreement is obtained with existing ab initio calculations from response theory in frequency domain [Luppi et al., Phys. Rev. B 82, 235201 (2010)]. We finally show applications to the second-harmonic generation of CdTe and the third-harmonic generation of Si.