The dielectric genome of van der Waals heterostructures

Abstract

Vertical stacking of two-dimensional (2D) crystals, such as graphene and hexagonal boron nitride, has recently lead to a new class of materials known as van der Waals heterostructures (vdWHs) with unique and highly tunable electronic properties. Abinitio calculations should in principle provide a powerful tool for modeling and guiding the design of vdWHs, but in their traditional, form such calculations are only feasible for commensurable structures with a few layers. Here we show that the dielectric properties of realistic, incommensurable vdWHs comprising hundreds of layers can be calculated with ab-initio accuracy using a multi-scale approach where the dielectric functions of the individual layers (the dielectric building blocks) are coupled simply via their long-range Coulomb interaction. We use the method to illustrate the 2D- 3D dielectric transition in multi-layer MoS2 crystals, the hybridization of quantum plasmons in large graphene/hBN heterostructures, and to demonstrate the intricate effect of substrate screening on the non-Rydberg exciton series in supported WS2.

To be published in Nano Lett

References in corpus (8)

• Light-emitting diodes by bandstructure engineering in van der Waals heterostructures
• Dielectric function, screening, and plasmons in 2D graphene
• Theory of surface plasmons and surface-plasmon polaritons
• Computational 2D Materials Database: Electronic Structure of Transition-Metal Dichalcogenides and Oxides
• Highly confined low-loss plasmons in graphene-boron nitride heterostructures
• Quasiparticle band structures and optical properties of strained monolayer MoS2 and WS2
• Linear density response function in the projector-augmented wave method: Applications to solids, surfaces, and interfaces
• MoS2: a Choice Substrate for Accessing and Tuning the Electronic Properties of Graphene

Cited by in corpus (88)

• The Computational 2D Materials Database: High-Throughput Modeling and Discovery of Atomically Thin Crystals
• Excitons in van der Waals heterostructures: The important role of dielectric screening
• Momentum-space indirect interlayer excitons in transition metal dichalcogenide van der Waals heterostructures
• GPAW: An open Python package for electronic-structure calculations
• Probing the influence of dielectric environment on excitons in monolayer WSe2: Insight from high magnetic fields
• Interlayer excitons and Band Alignment in MoS${}_2$/hBN/WSe${}_2$ van der Waals Heterostructures
• Simple Screened Hydrogen Model of Excitons in Two-Dimensional Materials
• Excitons versus electron-hole plasma in monolayer transition metal dichalcogenide semiconductors
• Dissociation of two-dimensional excitons in monolayer WSe2
• The dielectric impact of layer distances on exciton and trion binding energies in van der Waals heterostructures
• Defect Tolerant Monolayer Transition Metal Dichalcogenides
• Electronic polarizability as the fundamental variable in the dielectric properties of two-dimensional materials
• Environmentally-Sensitive Theory of Electronic and Optical Transitions in Atomically-Thin Semiconductors
• Rigid band shifts in two-dimensional semiconductors through environmental screening
• Cavity control of Excitons in two dimensional Materials
• Engineering of Neutral Excitons and Exciton Complexes in Transition Metal Dichalcogenide Monolayers through External Dielectric Screening
• Shedding Light on Moire Excitons: A First-Principles Perspective
• Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors
• Substrate screening effects on the quasiparticle band gap and defect charge transition levels in MoS${}_2$
• Electronic Structure Theory of Strained Two-Dimensional Materials with Hexagonal Symmetry
• Probing the local nature of excitons and plasmons in few-layer MoS2
• In Pursuit of 2D Materials for Maximum Optical Response
• Quantum embedding methods for correlated excited states of point defects: Case studies and challenges
• Influence of the effective layer thickness on the groundstate and excitonic properties of transition-metal dichalcogenide systems
• Designing in-plane heterostructures of quantum spin hall insulators from first principles: 1T'-MoS2 with adsorbates
• Competing Coulomb and electron-phonon interactions in NbS${}_2$
• Dependence of the hBN Layer Thickness on the Band Structure and Exciton Properties of Encapsulated WSe2 Monolayers
• Coexisting charge density wave and ferromagnetic instabilities in monolayer InSe
• Accelerating $GW$-Based Energy Level Alignment Calculations for Molecule-Metal Interfaces Using a Substrate Screening Approach
• Efficient Computational Design of 2D van der Waals Heterostructures: Band-Alignment, Lattice-Mismatch, Web-app Generation and Machine-learning
• Distinctive signatures of the spin- and momentum-forbidden dark exciton states in the photo-luminescences of strained WSe${}_2$ monolayers under thermalization
• Asymmetric Electric Field Screening in van der Waals Heterostructures
• Excitons in van der Waals materials: from monolayer to bulk hexagonal boron nitride
• Unified ab initio description of Fröhlich electron-phonon interactions in two-dimensional and three-dimensional materials
• Quasiparticle Levels at Large Interface Systems from Many-body Perturbation Theory: the XAF-GW method
• Prominent room temperature valley polarization in WS2/graphene heterostructures grown by chemical vapor deposition
• Combining density functional theory with macroscopic QED for quantum light-matter interactions in 2D materials
• Electrical control of inter-layer excitons in van der Waals heterostructures
• Nonconventional screening of Coulomb interaction in two-dimensional semiconductors and metals: A comprehensive cRPA study of MX2 (M=Mo, W, Nb, Ta; X=S, Se, Te)
• Electrostatics of electron-hole interactions in van der Waals heterostructures
• Phonon-limited Mobility of 2D Semiconductors: Quadrupole Scattering and Free-carrier Screening
• Ab initio calculations of quantum light-matter interactions in general electromagnetic environments
• Transferable screened range-separated hybrid functionals for electronic and optical properties of van der Waals materials
• Band nesting and exciton spectrum in monolayer MoS${}_2$
• Spin-orbit-proximitized ferromagnetic metal by monolayer transition metal dichalcogenide: Atlas of spectral functions, spin textures and spin-orbit torques in Co/MoSe${}_2$, Co/WSe${}_2$ and Co/TaSe${}_2$ heterostructures
• Optical Properties of Anisotropic Excitons in Phosphorene
• Anomalous Non-Hydrogenic Exciton Series in 2D Materials on High-$\kappa$ Dielectric Substrates
• Breakdown of the static dielectric screening approximation of Coulomb interactions in atomically thin semiconductors
• Interplay of screening and superconductivity in low-dimensional materials
• Plasmonics in Argentene
• Remote free-carrier screening to boost the mobility of Fröhlich-limited 2D semiconductors
• Strong two-dimensional plasmon in Li-intercalated hexagonal boron-nitride film with low damping
• Tin monochalcogenide heterostructures as mechanically rigid infrared bandgap semiconductors
• Microscopic model of the doping dependence of line widths in monolayer transition metal dichalcogenides
• Exciton spectrum in atomically thin monolayers: The role of hBN encapsulation
• Universal polarization energies for defects in monolayer, surface and bulk hexagonal boron nitride : A finite-size fragments GW approach
• Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2
• Tunable properties of excitons in double monolayer semiconductor heterostructures
• Computational methods for 2D materials modelling
• Spin-dependent Tunneling Barriers in CoPc/VSe2 from Many-Body Interactions
• Dielectric embedding GW for weakly coupled molecule-metal interfaces
• Screening Induced Crossover between Phonon- and Plasmon-Mediated Pairing in Layered Superconductors
• Layer Response Theory: Energetics of layered materials from semi-analytic high-level theory
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• High-throughput characterization of transition metal dichalcogenide alloys: Thermodynamic stability and electronic band alignment
• Two-dimensional excitons in monolayer transition metal dichalcogenides from simple models and variational calculations
• The reliability of hybrid functionals for accurate fundamental and optical gap prediction of bulk solids and surfaces
• Scaleability of dielectric susceptibility ${\epsilon }_{zz}$ with the number of layers and additivity of ferroelectric polarization in van der Waals semiconductors
• Quantum well confinement and competitive radiative pathways in the luminescence of black phosphorus layers
• Many-body $GW$ calculations with very large scale polarizable environments made affordable: a fully ab initio QM/QM approach
• Ab-initio calculations for electronic and optical properties of Er${}_{\mathrm{W}}$ defects in tungsten disulfide
• Probing the structure and composition of van der Waals heterostructures using the nonlocality of Dirac plasmons in the terahertz regime
• Advancing excited-state properties of two-dimensional materials using a dielectric-dependent hybrid functional
• Plasmonic Waveguides from Coulomb-Engineered Two-Dimensional Metals
• Excitonic insulators and superfluidity in 2D bilayers without external fields
• Quantized exciton-exciton annihilation in monolayer WS2 on SrTiO3 substrates with atomically flat terraces
• Tailoring a Molecule's Optical Absorbance Using Surface Plasmonics
• Ab-initio Van der Waals electrodynamics: polaritons and electron scattering from plasmons and phonons in BN-capped graphene
• First-principles computational methods for quantum defects in two-dimensional materials: A perspective
• Semiclassical theory for plasmons in two-dimensional inhomogeneous media
• Femtosecond concerted rotation of molecules on a 2D material interface
• Exciton Superfluidity in 2D Heterostructures from First Principles: The importance of material specific screening
• Extremely high excitonic $g$-factors in 2D crystals by alloy-induced admixing of band states
• Quantum plasmons with optical-range frequencies in doped few-layer graphene
• Understanding the Effects of Dielectric Property, Separation Distance, and Band Alignment on Interlayer Excitons in 2D Hybrid MoS2/WSe2 Heterostructures
• Device-scaling constraints imposed by the van der Waals gap formed in two-dimensional materials
• Radiative properties of quantum emitters in boron nitride from excited state calculations and Bayesian analysis
• Exact long-range dielectric screening and interatomic force constants in quasi-2D crystals