Understanding Interfaces of Molybdenum Disulfide and Ionic Liquids Using Electronic Structure Methods

The electrochemical gating of molybdenum disulfide (MoS₂) flakes with ionic liquids (ILs) offers opportunities in neuromorphic computing. Computational methods are leveraged to provide insights about the relationship between structure and electronic properties arising from MoS₂-IL interactions. DFT relaxation calculations, with continuum solvation effects and van der Waals approximations, were used to parse equilibrium configurations of both adsorbed and intercalated ion pairs within these systems and understand the atomic scale structure. Without Empty STates (WEST) GW-calculations were conducted on DFT-relaxed structures to accurately capture the dielectric constant as a function of frequency and space as a foundation to analyze the response to electric fields and optical excitation. Results are then corroborated with structure analysis using x-ray scattering and through the use of continuum modeling. This study will provide fundamental insights that can help guide the development of future materials for neuromorphic computing technologies.