论文标题

非局部伪能量密度的无轨道密度功能理论的功能

Nonlocal Pseudopotential Energy Density Functional for Orbital-Free Density Functional Theory

论文作者

Xu, Qiang, Ma, Cheng, Mi, Wenhui, Wang, Yanchao, Ma, Yanming

论文摘要

无轨道密度功能理论(DFT)以低计算成本运行,与模拟原子的数量线性缩放,使其适用于大规模材料模拟。通常认为,DFT严格要求使用局部伪电势,而不是轨道依赖性的非局部伪能力,以计算电子离子相互作用能量,因为没有轨道可用。这是不幸的情况,因为已知非局部伪电势可提供比本地的可传递性和计算精度更好的情况。我们在这里报告了一个理论方案的开发,该方案允许在DFT中直接使用非局部假ps。在此方案中,非局部假能量密度函数是通过非局部伪能力投影在非相互作用密度矩阵(而不是“轨道”)上的投影得出的,可以显式地将其作为电子密度的函数近似。我们的发展违反了这样一种信念,即非局部假性不适用于DFT,从而导致创建了DFT的替代理论框架,该框架比传统的框架优于传统框架。

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly requires the use of local pseudopotentials, rather than orbital-dependent nonlocal pseudopotentials, for the calculation of electron-ion interaction energies, as no orbitals are available. This is unfortunate situation since the nonlocal pseudopotentials are known to give much better transferability and calculation accuracy than local ones. We report here the development of a theoretical scheme that allows the direct use of nonlocal pseudopotentials in OF-DFT. In this scheme, a nonlocal pseudopotential energy density functional is derived by the projection of nonlocal pseudopotential onto the non-interacting density matrix (instead of 'orbitals') that can be approximated explicitly as a functional of electron density. Our development defies the belief that nonlocal pseudopotentials are not applicable to OF-DFT, leading to the creation of an alternate theoretical framework of OF-DFT that works superior to the traditional one.

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