High carrier mobility in organic cations intercalated multilayer MoS₂

Two-dimensional semiconductors, such as MoS2, have demonstrated great potential applications in post-Moore electronic and optoelectronic devices, and organic cations intercalation has been widely utilized to modulate their physical properties. However, the correlation between the conductivity, carrier mobility, carrier density, and structure of organic cations intercalated MoS2 is still unclear. In this Letter, we systematically investigated the structural and electrical transport properties of pristine MoS2 and MoS2 intercalated with various organic cations such as tetradecyltrimethyl-ammonium, tetraheptyl-ammonium, and cetyltrimethyl-ammonium. Semimetal bismuth (Bi) was used as electrodes to make Ohmic contact with MoS2, and four-probe measurements were employed to obtain the intrinsic conductivity of MoS2. The intercalated organic cations greatly expand interlayer spacing and strongly dope MoS2 up to an electron concentration of 6.1 x 10(13) cm(-2) depending on the size and intercalation amount of organic cations. The severe electron doping constrains the out-of-plane A(1g) vibration mode and screens the Coulomb scattering, such that the intercalated MoS2 has enhanced Hall mobility of >50 cm(2) V-1 s(-1) at room temperature and even >1700 cm(2) V-1 s(-1) at 5 K. The intercalated MoS2 responds much faster than pristine MoS2 when functioning as a phototransistor. Our work provides insight for understanding the electrical transport properties of MoS2 and designing more efficient electronic and optoelectronic devices.