Three-Dimensional Surface Treatment of MoS₂ Using BCl₃ Plasma-Derived Radicals

The realization of next-generation gate-all-around field-effect transistors (FETs) using two-dimensional transition metal dichalcogenide (TMDC) semiconductors necessitates the exploration of a three-dimensional (3D) and damage-free surface treatment method to achieve uniform atomic layer-deposition (ALD) of a high-k dielectric film on the inert surface of a TMDC channel. This study developed a BCl3 plasma-derived radical treatment for MoS2 to functionalize MoS2 surfaces for the subsequent ALD of an ultrathin Al2O3 film. Microstructural verification demonstrated a complete coverage of an approximately 2 nm-thick Al2O3 film on a planar MoS2 surface, and the applicability of the technique to 3D structures was confirmed using a suspended MoS2 channel floating from the substrate. Density functional theory calculations supported by optical emission spectroscopy and X-ray photoelectron spectroscopy measurements revealed that BCl radicals, predominantly generated by the BCl3 plasma, adsorbed on MoS2 and facilitated the uniform nucleation of ultrathin ALD–Al2O3 films. Raman and photoluminescence measurements of monolayer MoS2 and electrical measurements of a bottom-gated FET confirmed negligible damage caused by the BCl3 plasma-derived radical treatment. Finally, the successful operation of a top-gated FET with an ultrathin ALD–Al2O3 (∼5 nm) gate dielectric film was demonstrated, indicating the effectiveness of the pretreatment