skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Twist-Angle-Dependent Ultrafast Charge Transfer in MoS2-Graphene van der Waals Heterostructures

Journal Article · · Nano Letters

Vertically stacked transition metal dichalcogenide-graphene heterostructures provide a platform for novel optoelectronic applications with high photoresponse speeds. Photoinduced nonequilibrium carrier and lattice dynamics in such heterostructures underlie these applications but have not been understood. In particular, the dependence of these photoresponses on the twist angle, a key tuning parameter, remains elusive. Here, using ultrafast electron diffraction, we report the simultaneous visualization of charge transfer and electron–phonon coupling in MoS2-graphene heterostructures with different stacking configurations. We find that the charge transfer timescale from MoS2 to graphene varies strongly with twist angle, becoming faster for smaller twist angles, and show that the relaxation timescale is significantly shorter in a heterostructure as compared to a monolayer. These findings illustrate that twist angle constitutes an additional tuning knob for interlayer charge transfer in heterobilayers and deepen our understanding of fundamental photophysical processes in heterostructures, of importance for future applications in optoelectronics and light harvesting.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC); Strategic Priority Research Program of Chinese Academy of Sciences
Grant/Contract Number:
AC02-76SF00515; 61888102; 11834017; XDB30000000
OSTI ID:
1873515
Journal Information:
Nano Letters, Vol. 21, Issue 19; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (51)

Long-lived charge separation following pump-wavelength–dependent ultrafast charge transfer in graphene/WS 2 heterostructures journal February 2021
Photodetectors based on graphene, other two-dimensional materials and hybrid systems journal October 2014
Light absorption optimization in two-dimensional transition metal dichalcogenide van der Waals heterostructures journal January 2018
High Responsivity, Large-Area Graphene/MoS 2 Flexible Photodetectors journal September 2016
Band Alignment and Minigaps in Monolayer MoS 2 -Graphene van der Waals Heterostructures journal June 2016
Nonequilibrium Lattice Dynamics in Monolayer MoS 2 journal February 2021
Moiré heterostructures as a condensed-matter quantum simulator journal February 2021
Tuning On–Off Current Ratio and Field-Effect Mobility in a MoS 2 –Graphene Heterostructure via Schottky Barrier Modulation journal May 2014
Momentum-Resolved View of Electron-Phonon Coupling in Multilayer WSe 2 journal July 2017
2D materials and van der Waals heterostructures journal July 2016
Ultrafast low-energy electron diffraction in transmission resolves polymer/graphene superstructure dynamics journal July 2014
Van der Waals heterostructures and devices journal July 2016
Picosecond photoresponse in van der Waals heterostructures journal October 2015
Ultrafast dynamics in van der Waals heterostructures journal November 2018
Electronic Structure of Twisted Bilayers of Graphene/MoS 2 and MoS 2 /MoS 2 journal February 2015
Probing effect of electric field on photocarrier transfer in graphene-WS_2 van der Waals heterostructures journal January 2017
Tuning the electronic structure of monolayer graphene/ Mo S 2 van der Waals heterostructures via interlayer twist journal November 2015
Twist-angle modulation of exciton absorption in MoS 2 /graphene heterojunctions journal October 2019
Facile synthesis of pentacle gold–copper alloy nanocrystals and their plasmonic and catalytic properties journal July 2014
Vertical field-effect transistor based on graphene–WS2 heterostructures for flexible and transparent electronics journal December 2012
Auger Recombination in Chemical Vapor Deposition-Grown Monolayer WS 2 journal November 2016
Ultrafast non-radiative dynamics of atomically thin MoSe2 journal November 2017
Photoinduced charge transfer in transition metal dichalcogenide heterojunctions – towards next generation energy technologies journal January 2020
Decelerated Hot Carrier Cooling in Graphene via Nondissipative Carrier Injection from MoS 2 journal August 2020
Angle Dependence of Interlayer Coupling in Twisted Transition Metal Dichalcogenide Heterobilayers journal December 2020
Photocarrier generation from interlayer charge-transfer transitions in WS 2 -graphene heterostructures journal February 2018
Hot carrier photovoltaics in van der Waals heterostructures journal January 2021
Ultrafast graphene photodetector journal October 2009
Highly efficient hot electron harvesting from graphene before electron-hole thermalization journal November 2019
Interlayer electron–phonon coupling in WSe2/hBN heterostructures journal October 2016
Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films journal May 2013
Ultrafast formation of a transient two-dimensional diamondlike structure in twisted bilayer graphene journal October 2020
Van der Waals heterostructures journal July 2013
Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials journal July 2013
Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction journal September 2015
Erratum: Hybrid graphene tunneling photoconductor with interface engineering towards fast photoresponse and high responsivity journal October 2017
Charge Versus Energy Transfer in Atomically Thin Graphene-Transition Metal Dichalcogenide van der Waals Heterostructures journal January 2018
Pyridoxine induces glutathione synthesis via PKM2-mediated Nrf2 transactivation and confers neuroprotection journal February 2020
Filtering the photoluminescence spectra of atomically thin semiconductors with graphene journal March 2020
Electron-lattice energy relaxation in laser-excited thin-film Au-insulator heterostructures studied by ultrafast MeV electron diffraction journal September 2017
Ultrafast Photophysics of 2D Semiconductors and Related Heterostructures journal January 2020
Advances in highly doped upconversion nanoparticles journal June 2018
Ultrafast Band Structure Control of a Two-Dimensional Heterostructure journal May 2016
Microscopic nonequilibrium energy transfer dynamics in a photoexcited metal/insulator heterostructure journal November 2019
Spontaneous formation of structurally diverse membrane channel architectures from a single antimicrobial peptide journal November 2016
Unusual Exciton–Phonon Interactions at van der Waals Engineered Interfaces journal January 2017
Direct observation of minibands in a twisted graphene/WS 2 bilayer journal April 2020
Graphene/MoS 2 Hybrid Technology for Large-Scale Two-Dimensional Electronics journal May 2014
Electron dynamics in MoS 2 -graphite heterostructures journal January 2017
Modulating PL and electronic structures of MoS 2 /graphene heterostructures via interlayer twisting angle journal December 2017
Interlayer-State-Coupling Dependent Ultrafast Charge Transfer in MoS 2 /WS 2 Bilayers journal April 2017