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Herein, we quantitatively analyze the evolution of the subgap density of states (DOSs) for multilayered molybdenum disulfide (m-MoS2) field effect transistors (FETs) with bilayered SiNx/SiOx gate dielectrics under positive bias stress (PBS) and negative bias stress (NBS) by using optical charge-pumping capacitance-voltage spectroscopy. To decouple external gas ambient effects on device instability, hydrophobic fluoropolymers (cyclized transparent optical polymer; CYTOP) are employed for m-MoS2 FETs followed by the evaluation of subgap-DOSs in the devices for the respective PBS (or NBS). Through extraction of subgap-DOSs and their deconvolution with an analytical model of acceptor (or donor)-like states, it is shown that the device instability is closely correlated with state transitions of DOSs, corresponding to shallow (or midgap) levels for monosulfur vacancy (VS) (or disulfur vacancy (VS2)). Moreover, after PBS, the initial states of VS (0) (or HS2 (0)) transit toward VS (−1) (or HS2 (−1)) via electron trapping, whereas the transition toward VS (0) and HS2 (+1) during NBS is assessed from the initial VS (−1) and HS2 (0) states. Furthermore, technology computer-aided design (TCAD) simulation based on the extracted DOSs properly replicates the measured I-V characteristics of m-MoS2 FETs with (and without) CYTOP encapsulation. In this study, subgap-DOS characterization via optical charge pumping and validation of the quantitative evolution of subgap-DOSs suggest that this platform can be potentially beneficial for an in-depth understanding of the origins of device instability for transition metal dichalcogenide (MX2)-based FETs, where M is a transition metal and X is a chalcogenide.INDEX TERMS MoS2, field effect transistor, density of state (DOS), bias stress instability, TCAD simulation

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