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Title: Direct Measurement of the Tunable Electronic Structure of Bilayer MoS 2 by Interlayer Twist

Journal Article · · Nano Letters

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 ($$\bar{Γ}$$ 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 $$\bar{Γ}$$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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
SC00112704
OSTI ID:
1354330
Report Number(s):
BNL-112846-2016-JA
Journal Information:
Nano Letters, Vol. 16, Issue 2; ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

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Band engineering in twisted molybdenum disulfide bilayers journal April 2018
General theoretical description of angle-resolved photoemission spectroscopy of van der Waals structures journal April 2018
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Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS 2 /WSe 2 hetero-bilayers journal January 2017
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Momentum-space indirect interlayer excitons in transition-metal dichalcogenide van der Waals heterostructures text January 2018
General theoretical description of angle-resolved photoemission spectroscopy of van der Waals structures text January 2017
Momentum-space indirect interlayer excitons in transition metal dichalcogenide van der Waals heterostructures text January 2018
Direct observation of multiple rotational stacking faults coexisting in freestanding bilayer MoS2 journal August 2017