Tunable Interlayer Charge-transfer States in MoSe$_2$/WS$_2$ Moir\'e Superlattices
Abstract
Moir\'e superlattices formed by transition metal dichalcogenide (TMD) heterobilayers provide a versatile platform for studying strongly correlated electronic, excitonic, and topological phenomena in solids. In particular, angle-aligned MoSe/WS heterobilayers, which have a Type-I band alignment at zero vertical electric field, host rich correlated spin and charge physics. Here, combining large-scale first-principles calculations and optical reflection spectroscopy, we report a thorough study of the emergent moir\'e excitonic states and interlayer charge-transfer states in angle-aligned electron-doped MoSe/WS moir\'e superlattices. The moir\'e excitonic states serve as sensitive optical probes to the localization profile of doped electrons. We observe a series of interlayer charge-transfer transitions from n/n = 1 to 4 (where n denotes the moir\'e density) when the vertical electric field switches the heterostructure band alignment from Type-I to Type-II. By tuning the vertical electric field, we can precisely control the interlayer electron localization, realizing a Fermi-Hubbard model with a tunable charge-transfer band on an effective honeycomb lattice. Furthermore, Monte Carlo simulation of the doping dependence of the electric-field susceptibility predicts that multiple correlated charge-ordered states appear at both integer and fractional fillings. Our results provide a holistic understanding of the emergent optical excitations and the correlated charge-transfer states in electron-doped MoSe/WS moir\'e superlattices.
Keywords
Cite
@article{arxiv.2605.05571,
title = {Tunable Interlayer Charge-transfer States in MoSe$_2$/WS$_2$ Moir\'e Superlattices},
author = {Zheyu Lu and Jiahui Nie and Tianle Wang and Rwik Dutta and Ruishi Qi and Jingxu Xie and Can Uzundal and Jianghan Xiao and Ziyu Wang and Yibo Feng and Kenji Watanabe and Takashi Taniguchi and James R. Chelikowsky and Archana Raja and Steven G. Louie and Mit H. Naik and Michael P. Zaletel and Feng Wang},
journal= {arXiv preprint arXiv:2605.05571},
year = {2026}
}