Band Filling and Cross Quantum Capacitance in Ion-Gated Semiconducting Transition Metal Dichalcogenide Monolayers

Ionic liquid gated field-effect transistors (FETs) based on semiconducting transition metal dichalcogenides (TMDs) are used to study a rich variety of extremely interesting physical phenomena, but important aspects of how charge carriers are accumulated in these systems are not understood. We address these issues by means of a systematic experimental study of transport in monolayer MoSe$_2$ and WSe$_2$ as a function of magnetic field and gate voltage, exploring accumulated densities of carriers ranging from approximately 10$^{14}$ cm$^{-2}$ holes in the valence band to 4x10$^{14}$ cm$^{-2}$ electrons in the conduction band. We identify the conditions when the chemical potential enters different valleys in the monolayer band structure (the K and Q valley in the conduction band and the two spin-split K-valleys in the valence band) and find that an independent electron picture describes the occupation of states well. Unexpectedly, however, the experiments show very large changes in the device capacitance when multiple valleys are occupied that are not at all compatible with the commonly expected quantum capacitance contribution of these systems, $\textit{C}$$_Q$=$\textit{e}^2$/(d$\mu$/d$\textit{n}$). This unexpected behavior is attributed to the presence of a cross quantum capacitance, which originates from screening of the electric field generated by charges on one plate from charges sitting on the other plate. Our findings therefore reveal an important contribution to the capacitance of physical systems that had been virtually entirely neglected until now. (short abstract due to size limitations - full abstract in the manuscript)