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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.

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Unscrambling for Subgap Density-of-States in Multilayered MoS2 Field Effect Transistors under DC Bias Stress via Optical Charge-Pumping Capacitance-Voltage Spectroscopy