论文标题
模拟材料的光谱特性需要具有渐近电纠正的密度函数
Density functionals with asymptotic-potential corrections are required for the simulation of spectroscopic properties of materials
论文作者
论文摘要
鉴定了密度函数中渐近电位误差的校正五个影响，这些效应可显着改善涉及电荷转移特征的分子激发态的计算特性。新开发的材料科学计算方法用于证明这些影响如何在材料光谱中表现出来。将叶绿素a作为分子光谱法的范式，22种标志性材料作为3D材料光谱范式以及硝化己二硼的VN缺损作为一个范例，建立了连接。缺陷可以同样被认为是自然界中的“分子”和“材料”，因此桥接了分子和材料光谱的领域。得出的结论是，在大多数情况下，应通过计算相似但渐近校正的CAM-B3LYP功能来代替目前被视为准确计算材料光谱的标准的密度功能性HSE06，其中一些特定功能仅提供进一步的改进。
Five effects of correction of the asymptotic potential error in density functionals are identified that significantly improve calculated properties of molecular excited states involving charge-transfer character. Newly developed materials-science computational methods are used to demonstrate how these effects manifest in materials spectroscopy. Connection is made considering chlorophyll-a as a paradigm for molecular spectroscopy, 22 iconic materials as paradigms for 3D materials spectroscopy, and the VN- defect in hexagonal boron nitride as an example of the spectroscopy of defects in 2D materials pertaining to nanophotonics. Defects can equally be thought of as being "molecular" and "materials" in nature and hence bridge the realms of molecular and materials spectroscopies. It is concluded that the density functional HSE06, currently considered as the standard for accurate calculations of materials spectroscopy, should be replaced, in most instances, by the computationally similar but asymptotically corrected CAM-B3LYP functional, with some specific functionals for materials use only providing further improvements.
