论文标题
氢化单层MOS $ _2 $中的激发状态
Excited states in hydrogenated single-layer MoS$_2$
论文作者
论文摘要
我们使用基于第一原理密度 - 矩阵时间依赖性密度功能性理论(TDDFT)的方法来计算几个氢覆盖的单层MOS $ _2 $的激发光谱。我们的结果表明,完全氢化的系统是金属化的,而在低覆盖范围内,单层MOS $ _2 $的光谱包括自旋偏振部分填充的局部局部间隙状态。这些状态来自H原子的S轨道,它们与表面S原子倾斜。该系统的计算出的吸收光谱揭示了标准的激子峰,这对应于绑定的价循环和传导带电子,以及涉及中间隙电荷的激发峰。与原始的单层MOS $ _2 $一样,发现氢化系统激发子的结合能相对较大(几十MEV),使其实验检测功能易于进行氢化,并建议将氢化作为旋钮来调整单层MOS $ _2 $ $ _2 $的光学特性。重要的是,我们发现氢化以抑制可见光光致发光,这与实验观测一致。顺便说一句,我们将氢覆盖率的影响与周期表(最轻的金属),Li和Na的接下来两个元素的影响与单层MOS $ _2 $的光谱特性相比,这导致了N掺杂的非磁性半导体的形成,这些半导体不允许允许进行抗激元状态。
We calculate the excitation spectrum of single-layer MoS$_2$ at several hydrogen coverages by using a method based on first-principles Density-Matrix Time-Dependent Density-Functional Theory (TDDFT). Our results show that the fully hydrogenated system is metallic, while in the low-coverage limit the spectrum of single-layer MoS$_2$ includes spin-polarized partially filled localized mid-gap states. These states arise from s-orbitals of H atoms which make a tilted bond with the surface S atoms. The calculated absorption spectrum of the system reveals standard excitonic peaks, which correspond to the bound valence-band hole and conduction-band electron, as well as excitonic peaks that involve the mid-gap charges. As in the case of pristine single-layer MoS$_2$, binding energies of the excitons of the hydrogenated system are found to be relatively large (few tens of meV), making their experimental detection facile and suggesting hydrogenation as a knob for tuning the optical properties of single-layer MoS$_2$. Importantly, we find hydrogenation to suppress visible light photoluminescence, in agreement with experimental observations. As an aside, we contrast the effects of hydrogen coverage to that of the next two elements in the same column of the periodic table (the lightest metals), Li and Na, on the spectral properties of single-layer MoS$_2$ which lead instead to the formation of n-doped non-magnetic semiconductors that do not allow excitonic states.