Charge versus energy transfer in atomically-thin graphene-transition metal dichalcogenide van der Waals heterostructures

Abstract

Van der Waals heterostuctures, made from stacks of two-dimensional materials, exhibit unique light-matter interactions and are promising for novel optoelectronic devices. The performance of such devices is governed by near-field coupling through, e.g., interlayer charge and/or energy transfer. New concepts and experimental methodologies are needed to properly describe two-dimensional heterointerfaces. Here, we report on interlayer charge and energy transfer in atomically thin metal (graphene)/semiconductor (transition metal dichalcogenide (TMD, here MoSe${}_2$)) heterostructures using a combination of photoluminescence and Raman scattering spectroscopies. The photoluminescence intensity in graphene/MoSe${}_2$ is quenched by more than two orders of magnitude and rises linearly with the photon flux, demonstrating a drastically shortened ($\sim 1~\tr{ps}$) room temperature MoSe${}_2$ exciton lifetime. Key complementary insights are provided from analysis of the graphene and MoSe${}_2$ Raman modes, which reveals net photoinduced electron transfer from MoSe${}_2$ to graphene and hole accumulation in MoSe${}_2$. Remarkably, the steady state Fermi energy of graphene saturates at $290\pm 15~\tr{meV}$ above the Dirac point. This behavior is observed both in ambient air and in vacuum and is discussed in terms of band offsets and environmental effects. In this saturation regime, balanced photoinduced flows of electrons and holes may transfer to graphene, a mechanism that effectively leads to energy transfer. Using a broad range of photon fluxes and diverse environmental conditions, we find that the presence of net photoinduced charge transfer has no measurable impact on the near-unity photoluminescence quenching efficiency in graphene/MoSe${}_2$. This absence of correlation strongly suggests that energy transfer to graphene is the dominant interlayer coupling mechanism between atomically-thin TMDs and graphene.

arXiv commentPhysical Review X, in press. 14 pages, 7 figures, with supplemental material

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• Van der Waals heterostructures
• Raman spectroscopy as a versatile tool for studying the properties of graphene
• 2D materials and van der Waals heterostructures
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• Two-Dimensional Material Nanophotonics
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• Atomically thin p-n junctions with van der Waals heterointerfaces
• Ultrafast Charge Transfer in Atomically Thin MoS2/WS2 Heterostructures
• Observation of giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
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• Electrical Control of Two-Dimensional Neutral and Charged Excitons in a Monolayer Semiconductor
• Born-Oppenheimer Breakdown in Graphene
• Tuning the graphene work function by electric field effect
• Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
• Phonon and Raman scattering of two-dimensional transition metal dichalcogenides from monolayer, multilayer to bulk material
• Tightly bound excitons in monolayer WSe2
• Electric Field Effect Tuning of Electron-Phonon Coupling in Graphene
• Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides
• Symmetry-dependent phonon renormalization in monolayer MoS2 transistor
• Optical Separation of Mechanical Strain from Charge Doping in Graphene
• Photovoltaic effect in an electrically tunable van der Waals heterojunction
• k.p theory for two-dimensional transition metal dichalcogenide semiconductors
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• Atmospheric Oxygen Binding and Hole Doping in Deformed Graphene on a SiO2 Substrate
• Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics
• Picosecond photoresponse in van der Waals heterostructures
• Probing the Intrinsic Properties of Exfoliated Graphene: Raman Spectroscopy of Free-Standing Monolayers
• Electronic properties of the MoS2-WS2 heterojunction
• Snapshots of non-equilibrium Dirac carrier distributions in graphene
• Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
• Direct view on the ultrafast carrier dynamics in graphene
• Exciton-exciton annihilation in MoSe2 monolayers
• Energy Transfer from Individual Semiconductor Nanocrystals to Graphene
• High Responsivity, Large-Area Graphene/MoS2 Flexible Photodetectors
• Generation of photovoltage in graphene on a femtosecond time scale through efficient carrier heating
• Evidence for Fast Interlayer Energy Transfer in MoSe2/WS2 Heterostructures
• Nonlinear Photoluminescence in Atomically Thin Layered WSe2 Arising from Diffusion-Assisted Exciton-Exciton Annihilation
• Probing the influence of dielectric environment on excitons in monolayer WSe2: Insight from high magnetic fields
• Universal Distance-Scaling of Non-radiative Energy Transfer to Graphene
• Reduced dielectric screening and enhanced energy transfer in single and few-layer MoS2
• Raman Spectroscopy of Electrochemically-Gated Graphene Transistors: Geometrical Capacitance, Electron-Phonon, Electron-Electron, and Electron-Defect Scattering
• Resonance effects in the Raman scattering of mono- and few layers MoSe${}_2$
• Quasiparticle band-edge energy and band offsets of monolayer of molybdenum and tungsten chalcogenide
• Unified description of the optical phonon modes in $N$-layer MoTe${}_2$
• Anomalous Frequency Trends in MoS2 Thin Films Attributed to Surface Effects
• Distance Dependence of the Energy Transfer Rate From a Single Semiconductor Nanostructure to Graphene
• Single Defect Center Scanning Near-Field Optical Microscopy on Graphene
• Photogating of mono- and few-layer MoS2
• Ultrafast electronic read-out of diamond NV centers coupled to graphene
• Dielectric screening of the Kohn anomaly of graphene on hexagonal boron nitride
• Ultra-low power threshold for laser induced changes in optical properties of 2D Molybdenum dichalcogenides
• All-Optical Blister Test of Suspended Graphene Using Micro-Raman Spectroscopy
• Optical Probing of Electronic Interaction between Graphene and Hexagonal Boron Nitride

Cited by in corpus (22)

• Strained bubbles in van der Waals heterostructures as local emitters of photoluminescence with adjustable wavelength
• Oxidation of Monolayer WS${}_2$ in Ambient is a Photoinduced Process
• Electronic band structure of Two-Dimensional WS2/Graphene van der Waals Heterostructures
• Photoluminescence from Single-Walled MoS${}_2$ Nanotubes Coaxially Grown on Boron Nitride Nanotubes
• Room Temperature Valley Polarization and Coherence in Transition Metal Dichalcogenide-Graphene van der Waals Heterostructures
• Localized Excitons in NbSe${}_2$-MoSe${}_2$ Heterostructures
• Theory of optically induced Förster Coupling in van der Waals coupled Heterostuctures
• Interlayer coupling and ultrafast hot electron transfer dynamics in metallic VSe2/graphene van der Waals heterostructures
• Prominent room temperature valley polarization in WS2/graphene heterostructures grown by chemical vapor deposition
• Spin splitting and strain in epitaxial monolayer WSe${}_2$ on graphene
• Apparent Differences between Single Layer Molybdenum Disulfide Fabricated via Chemical Vapor Deposition and Exfoliation
• Large-area van der Waals epitaxy and magnetic characterization of Fe${}_3$GeTe${}_2$ films on graphene
• Narrow photoluminescence peak of epitaxial MoS${}_2$ on graphene/Ir(111)
• Impact of dark excitons on Förster type resonant energy transfer between dye molecules and atomically thin semiconductors
• Excitation-Dependent High-Lying Excitonic Exchange via Interlayer Energy Transfer from Lower-to-Higher Bandgap 2D Material
• Distance dependence of the energy transfer mechanism in WS${}_2$-graphene heterostructures
• Gate-tunable trion switch for excitonic device applications
• Graphene Oxide Photoreduction Recovers Graphene Hot Electron Cooling Dynamics
• Single- and narrow-line photoluminescence in a boron nitride-supported MoSe${}_2$/graphene heterostructure
• Manipulating single photon emitter radiative lifetime in transition-metal dichalcogenides through Forster resonance energy transfer to graphene
• Electrical Control of Excitons in Bare-MoSe2 and MoSe2/NbSe2 Heterostructure
• Graphene as a Tunable Nonradiative Bath for Moiré Excitons