Here, ultra‐long lifetimes of defect‐trapped single quantum emitters (SQEs) in monolayer WSe2/hBN heterostructures are reported. The lifetimes of these SQEs are approximately 225 ns, more than two orders of magnitude larger than what has been previously reported for defect‐trapped excitons in WSe2. These SQEs consist of co‐linearly polarized doublet peaks with a fine structure splitting of 0.45 meV. Second‐order correlation measurements show antibunched single‐photon emission with a g(2)(0) value of ≈0.13. Through numerical analysis and modeling, it is shown how such long‐lifetime single emitters can arise from bright and dark exciton coupling in antisite defects on the W sites. Additionally, high‐quality single‐photon emission over a wide range of lifetimes—from 2 ns to over 200 ns—is also reported, suggesting a variety of other possible defect structures present. The flexibility to generate high fidelity single‐photon emission, over a wide range of lifetimes in a single material system, has potential in many optical quantum computing applications from high‐bit‐rate single‐photon sources to quantum memory devices.
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.
more » « less- PAR ID:
- 10237153
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- npj Computational Materials
- Volume:
- 7
- Issue:
- 1
- ISSN:
- 2057-3960
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract -
Single-photon emitters serve as building blocks for many emerging concepts in quantum photonics. The recent identification of bright, tunable and stable emitters in hexagonal boron nitride (hBN) has opened the door to quantum platforms operating across the infrared to ultraviolet spectrum. Although it is widely acknowledged that defects are responsible for single-photon emitters in hBN, crucial details regarding their origin, electronic levels and orbital involvement remain unknown. Here we employ a combination of resonant inelastic X-ray scattering and photoluminescence spectroscopy in defective hBN, unveiling an elementary excitation at 285 meV that gives rise to a plethora of harmonics correlated with single-photon emitters. We discuss the importance of N π* anti-bonding orbitals in shaping the electronic states of the emitters. The discovery of elementary excitations in hBN provides fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.more » « less
-
more » « less
Abstract Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVVand spin qubits such as TiVVand MoVVin hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.
-
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
-
more » « less
Abstract Two‐dimensional (2D) hexagonal boron nitride (hBN) is one of the most promising candidates to host solid‐state single photon emitters (SPEs) for various quantum technologies. However, the 2D nature with an atomic‐scale thickness leads to inevitable challenges in spectral variability caused by substrate disturbance, lattice strain heterogeneity, and defect variation. Here, three‐dimensional (3D) nanoarchitectured hBN is reported with integrated SPEs from native defects generated during high‐temperature chemical vapor deposition (CVD). The 3D hBN has a quasi‐periodic gyroid minimal surface structure and is composed of a continuous 2D hBN sheet with built‐in convex and concave curvatures that promote the formation of optically active and thermally robust native defects. The free‐standing feature of the gyroid hBN with a nearly zero mean curvature can effectively eliminate the substrate disturbance and minimize lattice strain heterogeneity. As a result, naturally occurring defects with a narrow SPE spectral distribution can be created and activated as color centers in the 3D hBN, and the density of the SPEs can be tailored by CVD temperature.
