Air-stable doping of transition metal dichalcogenides is of fundamental importance to enable a wide range of optoelectronic and electronic devices while exploring their basic material properties. Here we demonstrate the use of benzyl viologen (BV), which has one of the highest reduction potentials of all electron-donor organic compounds, as a surface charge transfer donor for MoS2 flakes. The n-doped samples exhibit excellent stability in both ambient air and vacuum. Notably, we obtained a high electron sheet density of ~1.2 × 10(13) cm(-2), which corresponds to the degenerate doping limit for MoS2. The BV dopant molecules can be reversibly removed by immersion in toluene, providing the ability to control the carrier sheet density as well as selective removal of surface dopants on demand. By BV doping of MoS2 at the metal junctions, the contact resistances are shown to be reduced by a factor of >3. As a proof of concept, top-gated field-effect transistors were fabricated with BV-doped n(+) source/drain contacts self-aligned with respect to the top gate. The device architecture, resembling that of the conventional Si transistors, exhibited excellent switching characteristics with a subthreshold swing of ~77 mV/decade.

We report here the first degenerate n-doping of few-layer MoS2 and WSe2 semiconductors by surface charge transfer using potassium. High-electron sheet densities of ~1.0 × 10(13) cm(-2) and 2.5 × 10(12) cm(-2) for MoS2 and WSe2 are obtained, respectively. In addition, top-gated WSe2 and MoS2 n-FETs with selective K doping at the metal source/drain contacts are fabricated and shown to exhibit low contact resistances. Uniquely, WSe2 n-FETs are reported for the first time, exhibiting an electron mobility of ~110 cm(2)/V·s, which is comparable to the hole mobility of previously reported p-FETs using the same material. Ab initio simulations were performed to understand K doping of MoS2 and WSe2 in comparison with graphene. The results here demonstrate the need of degenerate doping of few-layer chalcogenides to improve the contact resistances and further realize high performance and complementary channel electronics.