论文标题
类似石墨烯的替代杂质的电子属性c $ _2 $ n,$ tg $ -c $ _3 $ n $ _4 $和$ hg $ -c $ -c $ _3 $ n $ _4 $
Electronic properties of substitutional impurities in graphene-like C$_2$N, $tg$-C$_3$N$_4$, and $hg$-C$_3$N$_4$
论文作者
论文摘要
我们研究了石墨型纳米多孔材料的替代杂质的电子和结构特性,c $ _2 $ n,$ tg $ - 和$ hg $ -c $ _3 $ n $ _4 $通过密度功能理论计算。我们考虑四种类型的杂质;碳位点上的硼取代(B(c)),氮位点上的碳取代(c(n)),碳位点上的氮取代(N(c))(n(c))以及氮位点上的硫取代(s(n))。从凝聚力计算中,我们发现C(n)和B(c)取代是最有利的,并且在杂质的附近诱导小键修改,而S(n)会诱导强烈的晶格失真。尽管所有研究的杂质都会在这些材料的带隙内诱导缺陷水平,但它们的电子特性取决于杂质作为受体或供体的行为。还观察到,受体(供体)波函数仅由杂质本身和/或相邻位点的$σ$($π$)轨道组成。因此,受体波函数针对孔,供体波形在整个相邻原子中更延伸,可以进一步探索该特性以修改这些材料与吸附物之间的相互作用。此外,杂质特性显示出强大的现场灵敏度和基态结合能,范围从$ 0.03 $到$ 1.13 $ eV,因此为调整这些材料的光学特性提供了有趣的路线。最后,自旋极化计算表明,所有杂质构型都具有磁接地状态,该磁场态由于杂质水平的自旋分裂而升高。在一些配置中,在GAP内可以找到一个以上的杂质水平,并且可能会探索两个杂质,以作为单光子发射的两级系统探索,此前最近在TMDC上对缺陷复合物提出了类似的建议。
We study the electronic and structural properties of substitutional impurities of graphenelike nanoporous materials C$_2$N, $tg$-, and $hg$-C$_3$N$_4$ by means of density functional theory calculations. We consider four types of impurities; boron substitution on carbon sites (B(C)), carbon substitution on nitrogen sites (C(N)), nitrogen substitution on carbon sites (N(C)), and sulfur substitution on nitrogen sites (S(N)). From cohesive energy calculations, we find that the C(N) and B(C) substitutions are the most energetically favorable and induce small bond modifications in the vicinity of the impurity, while the S(N) induces strong lattice distortions. Though all of the studied impurities induce defect levels inside the band gap of these materials, their electronic properties are poles apart depending on the behavior of the impurity as an acceptor or a donor. It is also observed that acceptor (donor) wavefunctions are composed only of $σ$ ($π$) orbitals from the impurity itself and/or neighboring sites. Consequently, acceptor wavefunctions are directed towards the pores and donor wavefunctions are more extended throughout the neighboring atoms, a property that could further be explored to modify the interaction between these materials and adsorbates. Moreover, impurity properties display a strong site sensitivity and ground state binding energies ranging from $0.03$ to $1.13$ eV, thus offering an interesting route for tuning the optical properties of these materials. Finally, spin-polarized calculations reveal that all impurity configurations have a magnetic ground state that rises from the spin splitting of the impurity levels. In a few configurations, more than one impurity level can be found inside the gap and two of them could potentially be explored as two-level systems for single-photon emission, following similar proposals recently made on defect complexes on TMDCs.