The stacking-dependent polarization and excitonic response of MoS$_2$/MoSe$_2$ heterostructures were investigated using GW+BSE many-body perturbation theory. While homobilayer MoS$_2$ exhibited a switchable interlayer dipole driven by registry-induced symmetry breaking, the MoS$_2$/MoSe$_2$ hetero-interface remained pinned by the intrinsic chemical potential mismatch between sulfur and selenium. In 2L-MoS$_2$/MoSe$_2$ trilayers, the stacking sequence enabled a deterministic control of photogenerated electrons between the central and bottom MoS$_2$ layers, governed by internal electric fields and quasiparticle band-edge shifts of 60--70~meV. Our calculations predicted a 36~meV interlayer excitonic shift, in remarkable agreement with recent experiments. These results elucidate the microscopic link between atomic registry and many-body interactions, establishing transition metal dichalcogenide trilayers as a potential platform for sliding ferroelectricity and programmable optoelectronic functionalities.
Light-Matter Interactions in Two-Dimensional Transition Metal Dichalcogenides: Dominant Excitonic Transitions in mono- and few-layer MoX$_2$ and Band Nesting
我们报告了基于Bethe Salpether方程+G $_0$ W $_0$的六个单和双层二硫属钼化合物的介电函数的从头计算，重点是激子跃迁占主导地位的吸收光谱的激发能为3\，eV。我们的计算表明，开关硫族元素原子和层间相互作用的强度应该影响的详细组成的高“C”峰的实验光谱的钼二硫族化物，并导致一个显着的自旋轨道分裂的贡献激子跃迁单层MoSe $_2$和MoTe $_2$。这可以通过沿着硫族元素系列S $\rightarrow$ Se $\rightarrow$ Te的费米能周围的电子色散的变化来解释，该变化沿着布里渊区中的\textit{$Γ$} - \textit{K}线移动二维材料的态密度中的范霍夫奇点。此外，我们确认了不同的层间特性的“\textsl{C}”峰过渡在几层的MoS $_2$，这是预测之前从实验数据，并表明，类似的行为可以预期MoSe $_2$和MoTe $_2$以及。
