Magnetic adatoms on properly designed surfaces constitute exquisite systems for addressing, controlling, and manipulating single quantum spins. Here, we show that monolayers of ${\mathrm{MoS}}_2$ on a Au(111) surface provide a versatile platform for controllably tuning the coupling between adatom spins and substrate electrons. Even for equivalent adsorption sites with respect to the atomic ${\mathrm{MoS}}_2$ lattice, we observe that Fe adatoms exhibit behaviors ranging from pure spin excitations, characteristic of negligible exchange and dominant single-ion anisotropy, to a fully developed Kondo resonance, indicating strong exchange and negligible single-ion anisotropy. This tunability emerges from a moiré structure of ${\mathrm{MoS}}_2$ on Au(111) in conjunction with pronounced many-body renormalizations. We also find striking spectral variations in the immediate vicinity of the Fe atoms, which we explain by quantum interference reflecting the formation of Fe-S hybrid states despite the nominally inert nature of the substrate. Our work establishes monolayer ${\mathrm{MoS}}_2$ as a tuning layer for adjusting the quantum spin properties over an extraordinarily broad parameter range. The considerable variability can be exploited for quantum spin manipulations.

中文翻译：

---

自旋激发的莫尔调谐：MoS2/Au(111) 上的单个 Fe 原子

设计合理的表面上的磁性吸附原子构成了用于寻址、控制和操纵单量子自旋的精致系统。在这里，我们表明单层${\mathrm{硫化钼}}_2$在 Au(111) 表面上提供了一个通用平台，用于可控地调整吸附原子自旋和衬底电子之间的耦合。即使对于相对于原子的等效吸附位点${\mathrm{硫化钼}}_2$在晶格中，我们观察到 Fe 吸附原子表现出的行为范围从纯自旋激发、可忽略不计的交换和主要的单离子各向异性，到完全发展的近藤共振，表明强交换和可忽略的单离子各向异性。这种可调性来自于${\mathrm{硫化钼}}_2$在 Au(111) 上结合明显的多体重整化。我们还在 Fe 原子附近发现了惊人的光谱变化，我们通过反映 Fe-S 杂化态形成的量子干涉来解释这一点，尽管基材名义上是惰性的。我们的工作建立了单层${\mathrm{硫化钼}}_2$作为用于在非常宽的参数范围内调整量子自旋特性的调谐层。相当大的可变性可用于量子自旋操作。