GW100: A Plane Wave Perspective for Small Molecules
GW100: A Plane Wave Perspective for Small Molecules
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DOI：
10.1021/acs.jctc.6b01150
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发表时间：
2017-02-01
影响因子：
5.5
通讯作者：
Kresse, Georg
中科院分区：
文献类型：
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作者：
Maggio, Emanuele;Liu, Peitao;Kresse, Georg
在最近的一项工作中，van Setten 和同事对 100 个闭壳分子进行了仔细收敛的 G(0)W(0) 研究 [J.化学。理论计算。 2015, 11, 5665-5687]。对于两种不同的代码，如果使用相同的高斯基组，他们发现在几个 10 meV 内有很好的一致性。我们使用投影仪增强波方法和维也纳从头算模拟软件包 (VASP) 检查同一组分子。对于电离势，基组外推平面波结果与高斯基组非常吻合，通常达到优于 50 meV 的一致性。为了实现这一一致性，我们纠正有限基组误差以及周期性重复图像引入的误差。对于正电子亲和势，高斯基组和 VASP 之间的差异稍大。我们将此归因于高斯基组的较大基组外推误差。然而，对于真空能级以上的准粒子 (QP) 共振，VASP 和高斯基组之间的差异很大。这可以暂时解释为高斯型轨道计算的基组收敛不足，如所选测试用例所示。
In a recent work, van Setten and co-workers have presented a carefully converged G(0)W(0) study of 100 closed shell molecules [J. Chem. Theory Comput. 2015, 11, 5665-5687]. For two different codes they found excellent agreement to within a few 10 meV if identical Gaussian basis sets were used. We inspect the same set of molecules using the projector augmented wave method and the Vienna ab initio simulation package (VASP). For the ionization potential, the basis set extrapolated plane wave results agree very well with the Gaussian basis sets, often reaching better than 50 meV agreement. In order to achieve this agreement, we correct for finite basis set errors as well as errors introduced by periodically repeated images. For positive electron affinities differences between Gaussian basis sets and VASP are slightly larger. We attribute this to larger basis set extrapolation errors for the Gaussian basis sets. For quasi particle (QP) resonances above the vacuum level, differences between VASP and Gaussian basis sets are, however, found to be substantial. This is tentatively explained by insufficient basis set convergence of the Gaussian type orbital calculations as exemplified for selected test cases.