Direct Measurement of the Tunable Electronic Structure of Bilayer MoS₂ by Interlayer Twist

Using angle-resolved photoemission on micrometer-scale sample areas, we directly measure the interlayer twist angle-dependent electronic band structure of bilayer molybdenum-disulfide (MoS₂). Our measurements, performed on arbitrarily stacked bilayer MoS₂ flakes prepared by chemical vapor deposition, provide direct evidence for a downshift of the quasiparticle energy of the valence band at the Brillouin zone center (Γ̅ point) with the interlayer twist angle, up to a maximum of 120 meV at a twist angle of ∼40°. Our direct measurements of the valence band structure enable the extraction of the hole effective mass as a function of the interlayer twist angle. While our results at Γ̅ agree with recently published photoluminescence data, our measurements of the quasiparticle spectrum over the full 2D Brillouin zone reveal a richer and more complicated change in the electronic structure than previously theoretically predicted. The electronic structure measurements reported here, including the evolution of the effective mass with twist-angle, provide new insight into the physics of twisted transition-metal dichalcogenide bilayers and serve as a guide for the practical design of MoS₂ optoelectronic and spin-/valley-tronic devices