Atomistic defect states as quantum emitters in monolayer MoS${}_2$

Abstract

Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum device technologies. The ability to tailor quantum emission through deterministic defect engineering is of growing importance for realizing scalable quantum architectures. However, a major difficulty is that defects need to be positioned site-selectively within the solid. Here, we overcome this challenge by controllably irradiating single-layer MoS${}_2$ using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion bombarded MoS${}_2$ flake with high-quality hBN reveals spectrally narrow emission lines that produce photons at optical wavelengths in an energy window of one to two hundred meV below the neutral 2D exciton of MoS${}_2$. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the helium ion bombardment. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and exotic Hubbard systems.

Main: 9 pages, 3 figures + SI: 19 pages, 10 figures

References in corpus (26)

• Atomically thin MoS2: A new direct-gap semiconductor
• Many-Body Physics with Ultracold Gases
• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Observation of giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
• Tightly bound excitons in monolayer WSe2
• Two-dimensional transition metal dichalcogenides under electron irradiation: defect production and doping
• Low-temperature photocarrier dynamics in monolayer MoS2
• Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics
• Large-scale quantum-emitter arrays in atomically thin semiconductors
• Deterministic strain-induced arrays of quantum emitters in a two-dimensional semiconductor
• Intrinsic Transport Properties of Electrons and Holes in Monolayer Transition Metal Dichalcogenides
• Stability and dopability of native defects and group-V and -VII impurities in single-layer MoS2
• Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory
• Quantum Dot Cavity-QED in the Presence of Strong Electron-Phonon Interactions
• Layer thickness-dependent phonon properties and thermal conductivity of MoS2
• Universal many-body response of heavy impurities coupled to a Fermi sea
• Defect-induced modification of low-lying excitons and valley selectivity in monolayer transition metal dichalcogenides
• The dielectric impact of layer distances on exciton and trion binding energies in van der Waals heterostructures
• Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
• A Waveguide-Coupled On-Chip Single Photon Source
• Theory of 2D crystals: graphene and beyond
• Discrete quantum dot like emitters in monolayer MoSe2: Spatial mapping, Magneto-optics and Charge tuning
• Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures
• On-chip generation, routing and detection of quantum light
• Coupling single photons from discrete quantum emitters in WSe${}_2$ to lithographically defined plasmonic slot-waveguides
• Robust valley polarization of helium ion modified atomically thin MoS${}_2$

Cited by in corpus (52)

• Irradiation of Nanostrained Monolayer WSe${}_2$ for Site-Controlled Single-Photon Emission up to 150 K
• Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride
• How Substitutional Point Defects in Two-Dimensional WS${}_2$ Induce Charge Localization, Spin-Orbit Splitting, and Strain
• Quantum Nanophotonics in Two-Dimensional Materials
• Prospects and challenges of quantum emitters in 2D materials
• Raman spectrum of Janus transition metal dichalcogenide monolayers WSSe and MoSSe
• Electrically driven photon emission from individual atomic defects in monolayer WS2
• The bright side of defects in MoS${}_2$ and WS${}_2$ and a generalizable chemical treatment protocol for defect passivation
• Nanomaterials for Quantum Information Science and Engineering
• Site-Controlled Telecom Single-Photon Emitters in Atomically-thin MoTe2
• Theory of exciton-electron scattering in atomically thin semiconductors
• Scalable single-photon sources in atomically thin MoS2
• Swing-up of quantum emitter population using detuned pulses
• Identifying defect-related quantum emitters in monolayer WSe${}_2$
• Roadmap for Photonics with 2D Materials
• Atomic Localization of Quantum Emitters in Multilayer Hexagonal Boron Nitride
• Sensing the local magnetic environment through optically active defects in a layered magnetic semiconductor
• Localized creation of yellow single photon emitting carbon complexes in hexagonal boron nitride
• Unveiling the Zero-Phonon Line of the Boron Vacancy Center by Cavity Enhanced Emission
• Vibronic response of a spin-1/2 state from a carbon impurity in two-dimensional WS${}_2$
• Spin-defect characteristics of single sulfur vacancies in monolayer ${\text{MoS}}_2$
• Lasing of Moiré Trapped MoSe${}_2$/WSe${}_2$ Interlayer Excitons Coupled to a Nanocavity
• Controlled defect production in monolayer MoS2 via electron irradiation at ultralow accelerating voltages
• Magnetic field imaging by hBN quantum sensor nanoarray
• Light-matter interaction in van der Waals heterostructures
• Effects of CVD Growth Parameters on Global and Local Optical Properties of MoS${}_2$ Monolayers
• Tuning the Optical Properties of an MoSe${}_2$ Monolayer Using Nanoscale Plasmonic Antennas
• Extrinsic localized excitons in patterned 2D semiconductors
• Selective-area van der Waals epitaxy of h-BN/graphene heterostructures via He${}^{+}$ irradiation-induced defect-engineering in 2D substrates
• Symmetry breaking and spin-orbit coupling for individual vacancy-induced in-gap states in MoS2 monolayers
• Thickness Insensitive Nanocavities for 2D Heterostructures using Photonic Molecules
• Plasmon Enhanced Quantum Properties of Single Photon Emitters with Hybrid Hexagonal Boron Nitride Silver Nanocube Systems
• Nonlocal Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS${}_2$ Monolayers
• Electronic Properties of Defective MoS${}_2$ Monolayers Subject to Mechanical Deformations: A First-Principles Approach
• Optical repumping of resonantly excited quantum emitters in hexagonal boron nitride
• Wigner Crystals in Two-Dimensional Transition-Metal Dichalcogenides: Spin Physics and Readout
• Plasmonic Nanocavity to Boost Single Photon Emission from Defects in Thin Hexagonal Boron Nitride
• Optical properties of MoSe${}_2$ monolayer implanted with ultra-low energy Cr ions
• Nano-optics of transition metal dichalcogenides and their van der Waals heterostructures with electron spectroscopies
• Creation and Microscopic Origins of Single-Photon Emitters in Transition Metal Dichalcogenides and Hexagonal Boron Nitride
• Quantum light generation with ultra-high spatial resolution in 2D semiconductors via ultra-low energy electron irradiation
• Comparative study of quantum emitter fabrication in wide bandgap materials using localized electron irradiation
• Signatures of Non-Markovianity in Cavity-QED with Color Centers in 2D Materials
• Effect of electron-irradiation on layered quantum materials
• Phonon-mediated exciton capture in Mo-based transition metal dichalcogenides
• Advancing the hBN Defects Database through Photophysical Characterization of Bulk hBN
• Ultra-Sensitive Extinction Measurements of Optically Active Defects in Monolayer MoS${}_2$
• Single charge control of localized excitons in heterostructures with ferroelectric thin films and two-dimensional transition metal dichalcogenides
• Effect of Interfacial Defects on the Electronic Properties of MoS${}_2$ Based Lateral T-H Heterophase Junctions
• Photo-physics and electronic structure of lateral graphene/MoS2 and metal/MoS2 junctions
• Comparison of the semiclassical and quantum optical field dynamics in a pulse-excited optical cavity with a finite number of quantum emitters
• Spin-valley qubits in gated quantum dots in a single layer of transition metal dichalcogenides