Point defects in hexagonal boron nitride (hBN) have attracted growing attention as bright single-photon emitters. However, understanding of their atomic structure and radiative properties remains incomplete. Here we study the excited states and radiative lifetimes of over 20 native defects and carbon or oxygen impurities in hBN using ab initio density functional theory and GW plus Bethe-Salpeter equation calculations, generating a large data set of their emission energy, polarization and lifetime. We find a wide variability across quantum emitters, with exciton energies ranging from 0.3 to 4 eV and radiative lifetimes from ns to ms for different defect structures. Through a Bayesian statistical analysis, we identify various high-likelihood charge-neutral defect emitters, among which the native VNNBdefect is predicted to possess emission energy and radiative lifetime in agreement with experiments. Our work advances the microscopic understanding of hBN single-photon emitters and introduces a computational framework to characterize and identify quantum emitters in 2D materials.
Color centers in hexagonal boron nitride (hBN) are presently attracting broad interest as a novel platform for nanoscale sensing and quantum information processing. Unfortunately, their atomic structures remain largely elusive and only a small percentage of the emitters studied thus far have the properties required to serve as optically addressable spin qubits. Here, we use confocal fluorescence microscopy at variable temperatures to study a new class of point defects produced via cerium ion implantation in thin hBN flakes. We find that, to a significant fraction, emitters show bright room-temperature emission, and good optical stability suggesting the formation of Ce-based point defects. Using density functional theory (DFT) we calculate the emission properties of candidate emitters, and single out the CeVBcenter—formed by an interlayer Ce atom adjacent to a boron vacancy—as one possible microscopic model. Our results suggest an intriguing route to defect engineering that simultaneously exploits the singular properties of rare-earth ions and the versatility of two-dimensional material hosts.
more » « less- NSF-PAR ID:
- 10305176
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Optical Materials Express
- Volume:
- 11
- Issue:
- 10
- ISSN:
- 2159-3930
- Page Range / eLocation ID:
- Article No. 3478
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Hexagonal boron nitride (hBN) has emerged as a promising ultrathin host of single photon emitters (SPEs) with favorable quantum properties at room temperature, making it a highly desirable element for integrated quantum photonic networks. One major challenge of using these SPEs in such applications is their low quantum efficiency. Recent studies have reported an improvement in quantum efficiency by up to two orders of magnitude when integrating an ensemble of emitters such as boron vacancy defects in multilayered hBN flakes embedded within metallic nanocavities. However, these experiments have not been extended to SPEs and are mainly focused on multiphoton effects. Here, the quantum single‐photon properties of hybrid nanophotonic structures composed of SPEs created in ultrathin hBN flakes coupled with plasmonic silver nanocubes (SNCs) are studied. The authors demonstrate 200% plasmonic enhancement of the SPE properties, manifested by a strong increase in the SPE fluorescence. Such enhancement is explained by rigorous numerical simulations where the hBN flake is in direct contact with the SNCs that cause the plasmonic effects. The presented strong and fast single photon emission obtained at room temperature with a compact hybrid nanophotonic platform can be very useful to various emerging applications in quantum optical communications and computing.
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Abstract Point defects in hexagonal boron nitride (hBN) are promising candidates as single-photon emitters (SPEs) in nanophotonics and quantum information applications. The precise control of SPEs requires in-depth understanding of their optoelectronic properties. However, how the surrounding environment of host materials, including the number of layers, substrates, and strain, influences SPEs has not been fully understood. In this work, we study the dielectric screening effect due to the number of layers and substrates, and the strain effect on the optical properties of carbon dimer and nitrogen vacancy defects in hBN from first-principles many-body perturbation theory. We report that environmental screening causes a lowering of the quasiparticle gap and exciton binding energy, leading to nearly constant optical excitation energy and exciton radiative lifetime. We explain the results with an analytical model starting from the Bethe–Salpeter equation Hamiltonian with Wannier basis. We also show that optical properties of quantum defects are largely tunable by strain with highly anisotropic response, in good agreement with experimental measurements. Our work clarifies the effect of environmental screening and strain on optoelectronic properties of quantum defects in two-dimensional insulators, facilitating future applications of SPEs and spin qubits in low-dimensional systems.more » « less
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Abstract Interlayer excitons (IXs) in MoSe2–WSe2heterobilayers have generated interest as highly tunable light emitters in transition metal dichalcogenide (TMD) heterostructures. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. We show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2–WSe2region to those in a region separated by bilayer hBN. The doping, electric field, and temperature dependence of the narrow IX lines are similar for both regions, but their excitonic g-factors have opposite signs, indicating that the origin of narrow IX PL is not the moiré potential.
