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The functionality of atomic quantum emitters is intrinsically linked to their host lattice coordination. Structural distortions that spontaneously break the lattice symmetry strongly impact their optical emission properties and spin-photon interface. Here we report on the direct imaging of charge state-dependent symmetry breaking of two prototypical atomic quantum emitters in mono- and bilayer MoS₂by scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM). By changing the built-in substrate chemical potential, different charge states of sulfur vacancies (Vac_S) and substitutional rhenium dopants (Re_Mo) can be stabilized. Vac$${}_{{{{{{{{\rm{S}}}}}}}}}^{-1}$$${}_S^{-1}$as well as Re$${}_{{{{{{{{\rm{Mo}}}}}}}}}^{0}$$${}_{\mathrm{Mo}}^0$and Re$${}_{{{{{{{{\rm{Mo}}}}}}}}}^{-1}$$${}_{\mathrm{Mo}}^{-1}$exhibit local lattice distortions and symmetry-broken defect orbitals attributed to a Jahn-Teller effect (JTE) and pseudo-JTE, respectively. By mapping the electronic and geometric structure of single point defects, we disentangle the effects of spatial averaging, charge multistability, configurational dynamics, and external perturbations that often mask the presence of local symmetry breaking.

Tailoring the electrical transport properties of two-dimensional transition metal dichalcogenides can enable the formation of atomically thin circuits. In this work, cyclic hydrogen and oxygen plasma exposures are utilized to introduce defects and oxidize MoS₂in a controlled manner. This results in the formation of sub-stochiometric MoO_3−x, which transforms the semiconducting behavior to metallic conduction. To demonstrate functionality, single flakes of MoS₂were lithographically oxidized using electron beam lithography and subsequent plasma exposures. This enabled the formation of atomically thin inverters from a single flake of MoS₂, which represents an advancement toward atomically thin circuitry.

The residue of common photo‐ and electron‐beam resists, such as poly(methyl methacrylate) (PMMA), is often present on the surface of 2D crystals after device fabrication. The residue degrades device properties by decreasing carrier mobility and creating unwanted doping. Here, MoS₂and WSe₂field effect transistors (FETs) with residue are cleaned by contact mode atomic force microscopy (AFM) and the impact of the residue on: 1) the intrinsic electrical properties, and 2) the effectiveness of electric double layer (EDL) gating are measured. After cleaning, AFM measurements confirm that the surface roughness decreases to its intrinsic state (i.e., ≈0.23 nm for exfoliated MoS₂and WSe₂) and Raman spectroscopy shows that the characteristic peak intensities (E_2gand A_1g) increase. PMMA residue causes p‐type doping corresponding to a charge density of ≈7 × 10¹¹cm⁻²on back‐gated MoS₂and WSe₂FETs. For FETs gated with polyethylene oxide (PEO)₇₆:CsClO₄, removing the residue increases the charge density by 4.5 × 10¹²cm⁻², and the maximum drain current by 247% (statistically significant,p< 0.05). Removing the residue likely allows the ions to be positioned closer to the channel surface, which is essential for achieving the best possible electrostatic gate control in ion‐gated devices.