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Transition metal dichalcogenide MoS2 is a two-dimensional material,attracting much attention for next-generation applications thanks to richfunctionalities stemmed from the crystal structure. Many experimental andtheoretical works have focused on the spin-orbit interaction which couples thevalley and spin degree of freedom so that the spin-states can be electricallycontrollable. However, the spin-states of charge carriers and vacancies havenot been yet elucidated directly from a microscopic viewpoint. We report thespin-states in thin-film electric double-layer transistors using operandoelectron spin resonance (ESR) spectroscopy. We have observed clearly differentESR signals of the conduction electrons and vacancies, and distinguished thecorresponding spin-states from the signals and theoretical calculations,evaluating the gate-voltage dependence and spin-susceptibility and g-factortemperature dependence. This analysis gives deep insight into the MoS2magnetism and clearly indicates the lower charge mobilities compared tographene, which would be useful for improvements of the device characteristicsand new applications.

MoS2 thin-film transistors spin-states, of conduction electrons and vacancies, distinguished by operando electron spin resonance