title: Twisted MoSe₂ Bilayers with Variable Local Stacking and Interlayer Coupling Revealed by Low-Frequency Raman Spectroscopy.
abstract: Unique twisted bilayers of MoSe2 with multiple stacking orientations and interlayer couplings in the narrow range of twist angles, 60 ± 3°, are revealed by low-frequency Raman spectroscopy and theoretical analysis. The slight deviation from 60° allows the concomitant presence of patches featuring all three high-symmetry stacking configurations (2H or AA', AB', and A'B) in one unique bilayer system. In this case, the periodic arrangement of the patches and their size strongly depend on the twist angle. Ab initio modeling predicts significant changes in frequencies and intensities of low-frequency modes versus stacking and twist angle. Experimentally, the variable stacking and coupling across the interface are revealed by the appearance of two breathing modes, corresponding to the mixture of the high-symmetry stacking configurations and unaligned regions of monolayers. Only one breathing mode is observed outside the narrow range of twist angles. This indicates a stacking transition to unaligned monolayers with mismatched atom registry without the in-plane restoring force required to generate a shear mode. The variable interlayer coupling and spacing in transition metal dichalcogenide bilayers revealed in this study may provide an interesting platform for optoelectronic applications of these materials.
authors.forename: Alexander A
authors.initials: AA
authors.lastname: Puretzky
authors.forename: Liangbo
authors.initials: L
authors.lastname: Liang
authors.forename: Xufan
authors.initials: X
authors.lastname: Li
authors.forename: Kai
authors.initials: K
authors.lastname: Xiao
authors.forename: Bobby G
authors.initials: BG
authors.lastname: Sumpter
authors.affiliation: Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , Troy, New York 12180, United States.
authors.forename: Vincent
authors.initials: V
authors.lastname: Meunier
authors.forename: David B
authors.initials: DB
authors.lastname: Geohegan
keywords: first-principles calculations; low-frequency Raman spectroscopy; stacking configurations; transition metal dichalcogenides; two-dimensional materials