大分子和纳米材料带电和中性激发能的简化GW/BSE方法
A simplified GW/BSE approach for charged and neutral excitation energies of large molecules and nanomaterials
摘要：
受Grimme的简化Tamm-Dancoff密度泛函理论方法的启发[S. Grimme，J. Chem. Phys. \textbf{138}，244104（2013）]中，我们描述了在GW近似下对自能和Bethe-Salpeter方程（BSE）进行激发态计算的简化方法，我们称之为sGW/sBSE。电子排斥积分的主要简化产生与张量超收缩相同的结构，使得我们的方法具有随系统大小二次增长的存储要求和随系统大小三次增长的计算时间。sGW的性能是在GW 100测试装置中对分子的电离势进行测试的，其与\textit{ab intio} GW的计算结果仅相差0.2 eV。sBSE（基于sGW输入）的性能在Thiel集合中的分子的激发能上进行测试，其中它与\textit{ab intio} GW/BSE计算相差约0.5 eV。作为系统的例子，可以常规研究与sGW/sBSE，我们计算的带隙和激发能的氢钝化硅纳米晶体与高达2650电子在4678空间轨道和吸收光谱的两个大的有机染料分子与数百个原子。
英文摘要：
Inspired by Grimme's simplified Tamm-Dancoff density functional theory approach [S. Grimme, J. Chem. Phys. \textbf{138}, 244104 (2013)], we describe a simplified approach to excited state calculations within the GW approximation to the self-energy and the Bethe-Salpeter equation (BSE), which we call sGW/sBSE. The primary simplification to the electron repulsion integrals yields the same structure as with tensor hypercontraction, such that our method has a storage requirement that grows quadratically with system size and computational timing that grows cubically with system size. The performance of sGW is tested on the ionization potential of the molecules in the GW100 test set, for which it differs from \textit{ab intio} GW calculations by only 0.2 eV. The performance of sBSE (based on sGW input) is tested on the excitation energies of molecules in the Thiel set, for which it differs from \textit{ab intio} GW/BSE calculations by about 0.5 eV. As examples of the systems that can be routinely studied with sGW/sBSE, we calculate the band gap and excitation energy of hydrogen-passivated silicon nanocrystals with up to 2650 electrons in 4678 spatial orbitals and the absorption spectra of two large organic dye molecules with hundreds of atoms.
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