Layered van der Waals materials are emerging as compelling two-dimensional platforms for nanophotonics, polaritonics, valleytronics and spintronics, and have the potential to transform applications in sensing, imaging and quantum information processing. Among these, hexagonal boron nitride (hBN) is known to host ultra-bright, room-temperature quantum emitters, whose nature is yet to be fully understood. Here we present a set of measurements that give unique insight into the photophysical properties and level structure of hBN quantum emitters. Specifically, we report the existence of a class of hBN quantum emitters with a fast-decaying intermediate and a long-lived metastable state accessible from the first excited electronic state. Furthermore, by means of a two-laser repumping scheme, we show an enhanced photoluminescence and emission intensity, which can be utilized to realize a new modality of far-field super-resolution imaging. Our findings expand current understanding of quantum emitters in hBN and show new potential ways of harnessing their nonlinear optical properties in sub-diffraction nanoscopy.

The assembly of quantum nanophotonic systems with plasmonic resonators is important for fundamental studies of single photon sources as well as for on-chip information processing. In this work, we demonstrate the controllable nanoassembly of gold nanospheres with ultra-bright narrow-band quantum emitters in 2D layered hexagonal boron nitride (hBN). We utilize an atomic force microscope (AFM) tip to precisely position gold nanospheres to close proximity to the quantum emitters and observe the resulting emission enhancement and fluorescence lifetime reduction. The extreme emitter photostability permits analysis at high excitation powers, and delineation of absorption and emission enhancement caused by the plasmonic resonators. A fluorescence enhancement of over 300% is achieved experimentally for quantum emitters in hBN, with a radiative quantum efficiency of up to 40% and a saturated count rate in excess of 5 106 counts per s. Our results are promising for the future employment of quantum emitters in hBN for integrated nanophotonic devices and plasmonic based nanosensors.

© 2017 Elsevier B.V. Optical properties of color centers in diamond have been the subject of intense research due to their promising applications in quantum photonics. In this work we study the optical properties of Xe related color centers implanted into nitrogen rich (type IIA) and an ultrapure, electronic grade diamond. The Xe defect has two zero phonon lines at 794 nm and 811 nm, which can be effectively excited using both green and red excitation, however, its emission in the nitrogen rich diamond is brighter. Near resonant excitation is performed at cryogenic temperatures and luminescence is probed under strong magnetic field. Our results are important towards the understanding of the Xe related defect and other near infrared color centers in diamond.

© 2017 American Chemical Society. Quantum emitters in layered hexagonal boron nitride (hBN) have recently attracted a great deal of attention as promising single photon sources. In this work, we demonstrate resonant excitation of a single defect center in hBN, one of the most important prerequisites for employment of optical sources in quantum information processing applications. We observe spectral line widths of an hBN emitter narrower than 1 GHz while the emitter experiences spectral diffusion. Temporal photoluminescence measurements reveal an average spectral diffusion time of around 100 ms. An on-resonance photon antibunching measurement is also realized. Our results shed light on the potential use of quantum emitters from hBN in nanophotonics and quantum information processing applications.

© 2017 Elsevier B.V. Remotely triggered drug delivery using nanoparticles is an area of great interest for targeted therapy to fight cancer. In this work, we synthesized photoresponsive nanoparticles to remotely initiate the delivery of doxorubicin (DOX) to 3D cultured human breast cancer cells (MCF-7) via NIR two-photon excitation (TPE) using nitrogen-doped and surface passivated (PEG 200 ) carbon nanohybrid dots (CNDs). On-demand drug delivery relies on bio-compatible, photo-responsive nano-carriers with high quantum yields. A facile (5 min synthesis) one-pot hot plate method was used to synthesize functionalized and surface passivated carbon nanohybrid dots (CND-P) having 53% quantum yield (QY). Compared to CNDs prepared from citric acid (CND-C) and citric acid plus urea (CND-N), CND-P had QY enhanced by factors of 12.6 and 4.4, respectively. The up-converted emission intensity of CND-P was strengthened by a factor of 4.5 over that of CND-N from nitrogen doped CNDs for similar test conditions (wavelength, excitation power and concentration). The drug loading capacity of CND-P was measured to be 0.98 w/w with the ability to release DOX via two-photon excitation (TPE). Intense green luminescence was observed under both 360 and 780 nm lasers using single and two-photon excitations. The highly biocompatible CND-P showed 88% cell viability at concentrations as high as 1100 µg/mL. The combined chemo- and photothermal therapeutic effect of the DOX-loaded CND-P (CND-P@DOX) complex resulted in the death of 78% of the MCF-7 cells compared to 59% with DOX alone.

Hexagonal boron nitride (hBN) has recently emerged as a fascinating platform for room-temperature quantum photonics due to the discovery of robust visible light single-photon emitters. In order to utilize these emitters, it is necessary to have a clear understanding of their atomic structure and the associated excitation processes that give rise to this single photon emission. Here, we performed density-functional theory (DFT) and constrained DFT calculations for a range of hBN point defects in order to identify potential emission candidates. By applying a number of criteria on the electronic structure of the ground state and the atomic structure of the excited states of the considered defects, and then calculating the Huang-Rhys (HR) factor, we found that the CBVN defect, in which a carbon atom substitutes a boron atom and the opposite nitrogen atom is removed, is a potential emission source with a HR factor of 1.66, in good agreement with the experimental HR factor. We calculated the photoluminescence (PL) line shape for this defect and found that it reproduces a number of key features in the experimental PL lineshape.

© 2017 American Chemical Society. Realization of quantum information and communications technologies requires robust, stable solid-state single-photon sources. However, most existing sources cease to function above cryogenic or room temperature due to thermal ionization or strong phonon coupling, which impedes their emissive and quantum properties. Here we present an efficient single-photon source based on a defect in a van der Waals crystal that is optically stable and oper ates at elevated temperatures of up to 800 K. The quantum nature of the source and the photon purity are maintained upon heating to 800 K and cooling back to room temperature. Our report of a robust high-temperature solid-state single photon source constitutes a significant step toward practical, integrated quantum technologies for real-world environments.

Arrays of fluorescent nanoparticles are highly sought after for applications in sensing, nanophotonics and quantum communications. Here we present a simple and robust method of assembling fluorescent nanodiamonds into macroscopic arrays. Remarkably, the yield of this directed assembly process is greater than 90% and the assembled patterns withstand ultra-sonication for more than three hours. The assembly process is based on covalent bonding of carboxyl to amine functional carbon seeds and is applicable to any material, and to non-planar surfaces. Our results pave the way to directed assembly of sensors and nanophotonics devices.