Observation of giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
arXiv:1404.2331 · doi:10.1038/nmat4061
Abstract
Two-dimensional (2D) transition metal dichalcogenides (TMDs) exhibit novel electrical and optical properties and are emerging as a new platform for exploring 2D semiconductor physics. Reduced screening in 2D results in dramatically enhanced electron-electron interactions, which have been predicted to generate giant bandgap renormalization and excitonic effects. Currently, however, there is little direct experimental confirmation of such many-body effects in these materials. Here we present an experimental observation of extraordinarily large exciton binding energy in a 2D semiconducting TMD. We accomplished this by determining the single-particle electronic bandgap of single-layer MoSe2 via scanning tunneling spectroscopy (STS), as well as the two-particle exciton transition energy via photoluminescence spectroscopy (PL). These quantities yield an exciton binding energy of 0.55 eV for monolayer MoSe2, a value that is orders of magnitude larger than what is seen in conventional 3D semiconductors. This finding is corroborated by our ab initio GW and Bethe Salpeter equation calculations, which include electron correlation effects. The renormalized bandgap and large exciton binding observed here will have a profound impact on electronic and optoelectronic device technologies based on single-layer semiconducting TMDs.
arXiv commentAccepted for publication in Nature Materials
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- Photodetection in p-n junctions formed by electrolyte-gated transistors of two-dimensional crystals
- Exotic dielectric behaviors induced by pseudo-spin texture in magnetic twisted bilayer
- Probing biexciton in monolayer WS through controlled many-body interaction
- Impacts of dielectric screening on the luminescence of monolayer WSe
- Many-body dynamics and gap opening in interacting periodically driven systems
- Band Gap Opening in Bilayer Graphene-CrCl/CrBr/CrI van der Waals Interfaces
- Probabilistic forecast of nonlinear dynamical systems with uncertainty quantification
- Annihilation mechanism of excitons in a MoS2 monolayer through direct Förster-type energy transfer and multistep diffusion
- Terahertz fingerprint of monolayer Wigner crystals
- Photophysical comparison of liquid and mechanically exfoliated WS monolayers
- Non-invasive control of excitons in two-dimensional materials
- Tunable properties of excitons in double monolayer semiconductor heterostructures
- High-throughput computational characterization of two-dimensional compositionally complex transition-metal chalcogenide alloys
- Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface
- Tightly bound excitons in two-dimensional semiconductors with a flat valence band
- Effect of dynamical screening in the Bethe-Salpeter framework: Excitons in crystalline naphthalene
- Screening 0D materials for 2D nanoelectronics applications
- Substrate Effect on Excitonic Shift and Radiative Lifetime of Two-Dimensional Materials
- Valley Depolarization in Monolayer Transition-Metal Dichalcogenides with Zone-Corner Acoustic Phonons
- Ultrafast creation of a light induced semimetallic state in strongly excited 1T-TiSe
- Excited-State Trions in Two Dimensional Materials
- Computing Optical Properties of Ultra-thin Crystals
- Torsional strain engineering of transition metal dichalcogenide nanotubes: An ab initio study
- Prevalence of oxygen defects in an in-plane anisotropic transition metal dichalcogenide
- Computational methods for 2D materials modelling
- Extremely imbalanced two-dimensional electron-hole-photon systems
- Chiral excitonics in monolayer semiconductors on patterned dielectric
- Confined monolayer Ag as a large gap 2D semiconductor and its momentum resolved excited states
- Dielectric screening at TMD:hBN interfaces: Monolayer-to-bulk transition, local-field effect, and spatial dependence
- Nano-optical investigation of grain boundaries, strain and edges in CVD grown MoS monolayers
- A comprehensive study of complex non-adiabatic exciton dynamics in MoSiN
- Spin-dependent Tunneling Barriers in CoPc/VSe2 from Many-Body Interactions
- Observation of Dynamic Screening in the Excited Exciton States in Multi-layered MoS
- Exciton diffusion in a hBN-encapsulated monolayer MoSe2
- Decoupling Molybdenum Disulfide from its Substrate by Cesium Intercalation
- Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response
- Dark-state impact on the exciton recombination of WS2 monolayers as revealed by multi-time-scale pump-and-probe spectroscopy
- Dielectric embedding GW for weakly coupled molecule-metal interfaces
- Trion clustering structure and binding energy in 2D semiconductor materials: Faddeev equations approach
- Vibrational and dielectric properties of monolayer transition metal dichalcogenides
- Van der Waals solid phase epitaxy to grow large-area manganese-doped MoSe few-layers on SiO/Si
- Growth of Thin Oxidation-Resistive Crystalline Si Nanostructures on Graphene
- The Exact Exchange-Correlation Potential in Time-Dependent Density Functional Theory: Choreographing Electrons with Steps and Peaks
- Interlayer excitonic spectra of vertically stacked MoSe/WSe heterobilayers
- Magneto photoluminescence measurements of tungsten disulphide monolayers
- Two-dimensional excitons in monolayer transition metal dichalcogenides from simple models and variational calculations
- Proximity induced spin-orbit splitting in graphene nanoribbons on transition metal dichalcogenides
- Reliable and Broad-range Layer Identification of Au-assisted Exfoliated Large Area MoS and WS Using Reflection Spectroscopic Fingerprints
- Valley Coherent Hot Carriers and Thermal Relaxation in Monolayer Transition Metal Dichalcogenides
- Nano-optics of transition metal dichalcogenides and their van der Waals heterostructures with electron spectroscopies
- Single-crystal graphene on Ir(110)
- Impact of substrates and quantum effects on exciton line shapes of 2D semiconductors at room temperature
- A Hybrid-DFT Study of Intrinsic Point Defects in (=Mo, W; =S, Se) Monolayers
- Exciton dissociation in two-dimensional transition metal dichalcogenides: Excited states and substrate effects
- Spatial control of carrier capture in two-dimensional materials: Beyond energy selection rules
- Valley-dependent Lorentz force and Aharonov-Bohm phase in strained graphene p-n junction
- Giant gate-tunable renormalization of spin-correlated flat-band states and bandgap in a 2D magnetic insulator
- Nearly-free-electron system of monolayer Na on the surface of single-crystal HfSe
- Triangular lattice exciton model
- Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides
- Elastic properties of Janus transition metal dichalcogenide nanotubes from first principles
- The deep-acceptor nature of the chalcogen vacancies in 2D transition-metal dichalcogenides
- Substrate screening approach for quasiparticle energies of two-dimensional interfaces with lattice mismatch
- A polarizing situation: Taking an in-plane perspective for next-generation near-field studies
- Isolating the Nonlinear Optical Response of a MoS Monolayer under Extreme Screening of a Metal Substrate
- First-principles calculations of electrical conductivities of edge-modified graphene nanoribbons: strain effect
- Magnetically tunable exciton valley coherence in monolayer WS mediated by the electron-hole exchange and exciton-phonon interactions
- Defects, band bending and ionization rings in MoS2
- Trion formation resolves observed peak shifts in the optical spectra of transition metal dichalcogenides
- Quantum many-body simulation using monolayer exciton-polaritons in coupled-cavities
- Phonon screening of excitons in atomically thin semiconductors
- Unveiling the multi-level structure of midgap states in Sb-doped MoX (X = S, Se, Te) monolayers
- Valley-contrasting interband transitions and excitons in symmetrically biased dice model
- Coulomb effects in the absorbance spectra of two-dimensional Dirac materials
- Interlayer and intralayer excitons in AlN/WS heterostructure
- Imaging Seebeck drift of excitons and trions in MoSe2 monolayers
- Phonons of electronic crystals in two-dimensional semiconductor moiré patterns
- Spin Response and Collective Modes in Simple Metal Dichalcogenides
- Layer-dependent Quasiparticle Electronic Structure of the P3HT:PCBM Interface from A First-Principles Substrate Screening Approach
- Controlling relaxation dynamics of excitonic states in monolayer transition metal dichalcogenides WS2 through interface engineering
- The Importance of Pure Dephasing in the Optical Response of Excitons in High-quality van der Waals Heterostructures
- Waveguiding valley excitons in monolayer transition metal dicalcogenides by dielectric interfaces in the substrate
- Modelling excitonic Mott transitions in two-dimensional semiconductors
- Thermal effect on magnetoexciton energy spectra in monolayer transition metal dichalcogenides
- Controlling Mixed Mo/MoS Domains on Si by Molecular Beam Epitaxy for the Hydrogen Evolution Reaction
- Coupled exciton internal and center-of-mass motions in two-dimensional semiconductors by a periodic electrostatic potential
- Many-body correlations brought to light in absorption spectra of diluted magnetic semiconductors
- Predicting the Energetic Stabilization of Janus-MoSSe/AlN Heterostructures: A DFT Study
- Femtosecond currents in transition metal dichalcogenides monolayers
- k-resolved ultrafast light-induced band renormalization in monolayer WS on graphene
- Persistence of charge ordering instability to Coulomb engineering in the excitonic insulator candidate TiSe
- Twistronics and moiré superlattice physics in 2D transition metal dichalcogenides
- Rich diversity of crystallographic phase formation in 2D Rex:Mo1-xS2 (x< 0.5) alloy
- Brightening odd-parity excitons in transition-metal dichalcogenides: Rashba spin-orbit interaction, skyrmions, and cavity polaritons
- Origin of selective enhancement of sharp defect emission lines in monolayer WSe on rough metal substrate
- Solving the Bethe-Salpeter equation on massively parallel architectures
- First-principles computational methods for quantum defects in two-dimensional materials: A perspective
- Phase transitions of polariton condensate in 2D Dirac materials
- Quasiparticle gap renormalization driven by internal and external screening in a WS device
- Interlayer Fermi polarons of excited exciton states in quantizing magnetic fields
- Alloying 2D VSe2 with Pt: from a charge density wave state to a disordered insulator
- Optical properties of orthorhombic germanium sulfide: Unveiling the Anisotropic Nature of Wannier Exciton
- Moiré induced electronic structure modifications in monolayer VS on Au(111)
- Quasiparticle Electronic Structure of Two-Dimensional Heterotriangulene-Based Covalent Organic Frameworks Adsorbed on Au(111)
- Dichotomy of saddle points in energy bands of a monolayer NbSe
- Robust Coulomb Gap and Varied-temperature Study of Epitaxial 1T'-WSe Monolayers
- Room-Temperature Quantum-Confined Stark Effect in Atomically Thin Semiconductor
- Electron-Doping Induced Semiconductor to Metal Transitions in ZrSe2 Layers via Copper Atomic Intercalation
- Symmetry-breaking and spin-blockage effects on carrier dynamics in single-layer tungsten diselenide
- Robustness of momentum-indirect interlayer excitons in MoS2/WSe2 heterostructure against charge carrier doping
- Motion of 2D exciton in momentum space leads to pseudospin distribution narrowing on the Bloch Sphere
- Low-Temperature Annihilation Rate for Quasi-Localized Excitons in Monolayer MoS2
- Spin dynamics of hot excitons in diluted magnetic semiconductors with spin-orbit interaction
- Strain-induced exciton decomposition and anisotropic lifetime modulation in a GaAs micromechanical resonator
- Valley-dependent emission patterns enabled by plasmonic nanoantennas
- Signatures of valley drift in the diversified band dispersions of bright, gray, and dark excitons in MoS2 monolayers under uni-axial strains
- Dimensionality-suppressed chemical doping in 2D semiconductors: the cases of phosphorene, MoS2, and ReS2 from first-principles
- Correspondence between quasiparticle dissipation and quantum information decay in open quantum systems
- Macroscopic electro-optical modulation of solution-processed molybdenum disulfide
- Retrieval of fundamental material parameters of monolayer transition metal dichalcogenides from experimental exciton energies: An analytical approach
- Designable exciton mixing through layer alignment in WS-graphene heterostructures
- Microring Resonators Coupling Tunability by Heterogeneous 2D Material Integration
- Ultrafast Terahertz Probe of Transient Evolution of Charged and Neutral Phase of Photoexcited Electron-hole Gas in Monolayer Semiconductor
- Direct observation of internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe_2
- Role of excited states in the dynamics of excitons and their spins in diluted magnetic semiconductors
- Coulomb potential screening via charged carriers and charge-neutral dipoles/excitons in two-dimensional case
- Variational and field-theoretical approach to exciton-exciton interactions and biexcitons in semiconductors
- Renormalization of the optical band gap through an effective Thirring interaction for massive Dirac-like electrons
- Ferroelectric Control of Interlayer Excitons in 3R-MoS / MoSe Heterostructures
- Substrate pre-sputtering for layer-by-layer van der Waals epitaxy of 2D materials
- Substrate Induced Optical Anisotropy in Monolayer MoS
- Gate-modulated reflectance spectroscopy for detecting excitonic species in two-dimensional semiconductors
- Nano-optical imaging of monolayer MoSe2-WSe2 lateral heterostructure
- Observation of the Interlayer Exciton Gases in WSe -p: WSe Heterostructures
- Valley-Selective Response of Nanoantennas Coupled to 2D Transition Metal Dichalcogenides
- Emergent exotic chirality dependent dielectricity in magnetic twisted bilayer system
- Momentum resolved ground/excited states and the ultra-fast excited state dynamics of monolayer MoS2
- Deciphering the Intense Post-Gap Absorptions of Monolayer Transition Metal Dichalcogenides
- Steady-state nonlinear optical response of excitons in monolayer MoSe
- Experimental valley qubit state tomography and coherence induced uncertainty relations in monolayer WSe
- Bandgap closing at the screw dislocations of WS2 spirals
- Loss and Coupling Tuning via Heterogeneous Integration of MoS2 Layers in Silicon Photonics
- Ab initio Approach to Collective Excitations in Excitonic Insulators
- Room-temperature tuning and probing of Fermi polarons in atomically thin semiconductors on a plasmonic metasurface
- Subnanometric control of coupling between WS monolayers with a molecular spacer
- Low-dimensional quantum systems