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© 2021, The Author(s). The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellitesʼ photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

The ability to control excitons in semiconductors underlies numerous proposed applications, from excitonic circuits to energy transport. Two dimensional (2D) semiconductors are particularly promising for room-temperature applications due to their large exciton binding energy and enormous stretchability. Although the strain-induced static exciton flux has been observed in predetermined structures, dynamic control of exciton flux represents an outstanding challenge. Here, we introduce a method to tune the bandgap of suspended 2D semiconductors by applying a local strain gradient with a nanoscale tip. This strain allows us to locally and reversibly shift the exciton energy and to steer the exciton flux over micrometer-scale distances. We anticipate that our result not only marks an important experimental tool but will also open a broad range of new applications from information processing to energy conversion., United States. Army Research Office. Multidisciplinary University Research Initiative (Grant W911NF-18-1-0431), National Science Foundation (U.S.). Emerging Frontiers & Multidisciplinary Activities. Quantum Optoelectronics, Magnetoelectronics and Plasmonics in 2-Dimensional Materials Heterostructures (Award Abstract 1542863), CREST (Grant JPMJCR15F3)

Single photon sources based on atomic defects in layered hexagonal boron nitride (hBN) have emerged as promising solid state quantum emitters with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structure of emitters as well as the coupling of their spin- and charge-dependent electronic states to phonons. Here, we investigate these questions using photoluminescence excitation (PLE) experiments at T = 4 K on single-photon emitters in multilayer hBN grown by chemical vapor deposition. By scanning up to 250 meV from the zero phonon line (ZPL), we can precisely measure the emitter's coupling efficiency to different phonon modes. Our results show that excitation mediated by the absorption of one in-plane optical phonon increases the emitter absorption probability 10-fold compared to that mediated by acoustic or out-of-plane optical phonons. We perform complementary theoretical predictions by first-principles density-functional theory of four defect candidates for which we calculate prevalent charge states and their spin-dependent coupling to bulk and local phonon modes. We discuss possible hypotheses to overcome the disparity between experimental results and theoretical predictions. Our work illuminates the phonon-coupled dynamics in hBN quantum emitters at cryogenic temperature, with implications more generally for mesoscopic quantum emitter systems in 2D materials, and represents possible applications in solid-state quantum technologies., United States. Army Research Office. Multidisciplinary University Research Initiative (Grant W911NF-18-1-0431)

Solid-state quantum emitters (QEs) are fundamental in photonic-based quantum information processing. There is strong interest to develop high-quality QEs in III-nitride semiconductors because of their sophisticated manufacturing driven by large and growing applications in optoelectronics, high voltage power transistors, and microwave amplifiers. Here, the generation and direct integration of QEs in an aluminum nitride-based photonic integrated circuit platform is reported. For individual waveguide-integrated QEs, an off-chip count rate exceeding 6 × 104 counts per second (cps; saturation rate >8.6 × 104 cps) is measured at room temperature under continuous-wave (CW) excitation. In an unpatterned thin-film sample, antibunching with g(2)(0) ∼0.08 and photon count rates exceeding 8 × 105 cps (saturation rate >1 × 106 cps) are measured at room temperature under CW excitation. Although spin and detailed optical line width measurements are left for future work, these results already show the potential for high-quality QEs monolithically integrated in a wide range of III-nitride device technologies that would enable new quantum device opportunities and industrial scalability., United States. Army Research Office MURI ((Ab-Initio Solid-State Quantum Materials Grant W911NF-18-1-0431), National Science Foundation (U.S.). Research Advanced by Interdisciplinary Science and Engineering (Grant CHE-1839155), Air Force Research Laboratory. RITA program ( FA8750-16-2-0141), National Research Foundation of Korea (Grants 2015R1A6A3A03020926 and 2018R1D1A1B07043390)

Bio-imaging requires robust ultra-bright probes without causing any toxicity to the cellular environment, maintain their stability and are chemically inert. In this work we present hexagonal boron nitride (hBN) nanoflakes which exhibit narrowband ultra-bright single photon emitters. The emitters are optically stable at room temperature and under ambient environment. hBN has also been noted to be noncytotoxic and seen significant advances in functionalization with biomolecules. We further demonstrate two methods of engineering this new range of extremely robust multicolour emitters across the visible and near infrared spectral ranges for large scale sensing and biolabeling applications.

Hexagonal boron nitride (hBN) is an emerging two-dimensional material for quantum photonics owing to its large bandgap and hyperbolic properties. Here we report two approaches for engineering quantum emitters in hBN multilayers using either electron beam irradiation or annealing and characterize their photophysical properties. The defects exhibit a broad range of multicolor room-temperature single photon emissions across the visible and the near-infrared spectral ranges, narrow line widths of sub-10 nm at room temperature, and a short excited-state lifetime, and high brightness. We show that the emitters can be categorized into two general groups, but most likely possess similar crystallographic structure. Remarkably, the emitters are extremely robust and withstand aggressive annealing treatments in oxidizing and reducing environments. Our results constitute a step toward deterministic engineering of single emitters in 2D materials and hold great promise for the use of defects in boron nitride as sources for quantum information processing and nanophotonics., National Science Foundation (U.S.) (Award 1542863)

Two-dimensional van der Waals materials have emerged as promising platforms for solid-state quantum information processing devices with unusual potential for heterogeneous assembly. Recently, bright and photostable single photon emitters were reported from atomic defects in layered hexagonal boron nitride (hBN), but controlling inhomogeneous spectral distribution and reducing multi-photon emission presented open challenges. Here, we demonstrate that strain control allows spectral tunability of hBN single photon emitters over 6 meV, and material processing sharply improves the single photon purity. We observe high single photon count rates exceeding 7 × 10 6 counts per second at saturation, after correcting for uncorrelated photon background. Furthermore, these emitters are stable to material transfer to other substrates. High-purity and photostable single photon emission at room temperature, together with spectral tunability and transferability, opens the door to scalable integration of high-quality quantum emitters in photonic quantum technologies., United States. Department of Energy. Office of Basic Energy Sciences (Award DE-SC0001088)