Atom-like defects in hexagonal boron nitride (hBN) provide room-temperature single-photon emission and coherent spin states, making them attractive for quantum-computing and -sensing applications. However, their random spatial and spectral characteristics hamper deterministic coupling with nano-optical cavities, limiting their use as bright single-photon sources and sensitive quantum sensors. Here, we present tip-enhanced quantum-sensing spectroscopy of single-photon emitters in hBN. Through precise spatial positioning of individual emitters within tip-cavities with different plasmon resonances, we adaptively control the enhancement rates of both excitation and emission, as well as the single-photon purity. In this way, optimal selection of their relative contributions can effectively reconfigure solid-state single-photon sources, with simultaneous nano-spectroscopic space- and time-resolved analyses. Furthermore, we demonstrate tip-enhanced quantum-sensing with single spin defects through optically detected magnetic resonance (ODMR) experiments in tip-coupled hBN nanoflakes. Our approach provides a unique pathway toward highly-sensitive and deterministic quantum-sensing with room-temperature single-photon emitters.
Atom-like defects in hexagonal boron nitride (hBN) provide room-temperature single-photon emission and coherent spin states, making them attractive for quantum-computing and -sensing applications. However, their random spatial and spectral characteristics hamper deterministic coupling with nano-optical cavities, limiting their use as bright single-photon sources and sensitive quantum sensors. Here, we present tip-enhanced quantum-sensing spectroscopy of single-photon emitters in hBN. Through precise spatial positioning of individual emitters within tip-cavities with different plasmon resonances, we adaptively control the enhancement rates of both excitation and emission, as well as the single-photon purity. In this way, optimal selection of their relative contributions can effectively reconfigure solid-state single-photon sources, with simultaneous nano-spectroscopic space- and time-resolved analyses. Furthermore, we demonstrate tip-enhanced quantum-sensing with single spin defects through optically detected magnetic resonance (ODMR) experiments in tip-coupled hBN nanoflakes. Our approach provides a unique pathway toward highly-sensitive and deterministic quantum-sensing with room-temperature single-photon emitters.
Optically addressable spin defects in hexagonal boron nitride (hBN) are well suited for near-surface quantum sensing. They offer bright, wavelength-tunable single-photon emission with high optically detected magnetic resonance (ODMR) contrast at room temperature. Here we controllably synthesise a high density of spin-complex defects in carbon-doped hBN flakes. We find that the zero-field splitting parameter D is directly correlated with the zero-phonon line of an emitter, while the ODMR contrast shows no such correlation. We further analyse an individual narrowband defect showing 68% ODMR contrast and enhance its photon collection by ~40% using a solid immersion lens. By advancing both the practical synthesis of the spin complexes and the understanding of their microscopic origin, our results move us toward the deterministic creation of ODMR-active quantum emitters
Single-photon sources are crucial components for building quantum networks and communications, but their optical coherent control remains a significant challenge in the development of quantum technologies. Recently, single-photon sources in atomically thin 2D materials such as transition metal dichalcogenides and van der Waals materials have emerged as promising solid-state quantum light emitters [1]. Hexagonal boron nitride (hBN) is a 2D insulator, which hosts optically active states in its band gap that efficiently emit single photons even at room temperature. The wide range of emission wavelengths, narrow emission lines, and convenient tunability of these hBN emitters make them particularly interesting for quantum sensing and wavelength division multiplexed quantum communications. They can also be found in commercially available nanocrystals, making them ideal for creating large arrays of single-photon emitters [2] and efficient coupling to photonic structures, such as 3D-printed microlenses [3].
Single photons are the key ingredient for many photonic quantum technologies including quantum key distribution and measurement-based quantum computing. However, it remains difficult to create devices with the appropriate specifications for use in non-laboratory environments. The optical microcavity platform provides an attractive route towards a room temperature single photon source device. Our ultra-small focused ion beam (FIB) milled open-access cavities offer enhancement of the spontaneous emission rate, tunability of the emission spectrum and increased light collection. The embedment of solid-state emitters within these cavities enables us to create a robust room temperature single photon source device, with the potential for high efficiencies and single photon purities. Defects such as the nitrogen-vacancy (NV) centre in diamond have been shown to be stable room-temperature sources of single photons. There are new single emitters emerging in two-dimensional materials such as hexagonal boron nitride (hBN). Here we present developments in room-temperature coupling of single defects to open-access microcavities of a planar-hemispherical geometry with mode volumes down to λ3. We report enhancements in the spectral density of photons into a single cavity mode, combined with improved single photon purities. It will be shown that the NV-cavity system provides a ~3% single photon emission efficiency with purities of up to 94%. The hBN-cavity system provides count rates >1Mcts/s into a single cavity mode with purities up to 96%. With these high single photon purities, such devices would be robust against photon number splitting attacks making them attractive for applications in quantum cryptography.
Room temperature solid-state emitters provide a promising source of single photons for use in quantum technologies. The emitters studied in this thesis are the nitrogen-vacancy (NV) centre in diamond, and defects in two-dimensional hexagonal boron nitride (hBN). In this thesis, I present investigations into the coupling of these defects to open-access microcavities at room temperature. The optical microcavity serves to confine the electric field down to mode volumes on the order of λ3, increasing the spontaneous emission rate of these emitters and channelling this emission into well defined cavity modes. The general properties of both emitters will be presented, including examples of single photon emission, emission spectra, saturation behaviour and photo-stability. A few examples highlighting the long-term photo-stability of the NV centre under pulsed excitation will be displayed. This will highlight the suitability of the NV centre for a practical device. Following the preparation and characterisation of each emitter, single photon emission into the cavity modes is verified, reaching single photon purities greater than 97%. Enhancements in the spectral density of photons were observed for both the NV centre (~25×) and defect in hBN (~3×), along with decreases in the excited state lifetimes. While the NV centre provides a stable source of single photons, the cavity enhancement is limited by its broad emission spectrum. Defects in hBN present near-ideal optical properties in the absence of the cavity, and were expected to deliver superior results within the cavity. However, the poor photo-stability of these defects did not allow complete characterisation of the cavity coupled emission. FDTD simulations were combined with changes in the excited state lifetime to infer the quantum efficiency of these defects. The results of this thesis form the foundation for the realisation of a robust room temperature single photon source.
Optical quantum technology needs efficient sources for non-classical light. Solid-state emitters provide excellent mode purity, high brightness, and often also stable operation up to room temperature. At the same time the spin of individual impurities can be entangled with emitted photons. Nano-photonic structures can dramatically enhance the photon emission efficiency and thus the yield of quantum information processing tasks involving photons. One example is a node of a quantum repeater network. In this presentation we address the issue of enhanced photon collection from optically active defects in the solid-state such as diamond [1] or two-dimensional material [2]. We briefly introduce the emitters and then describe recent experiments where we couple them to dielectric/plasmonic antennas [3] and to SiO2/Si light collecting structures [4]. References [1] “Fiber-Coupled Diamond Micro-Waveguides toward an Efficient Quantum Interface for Spin Defect Centers”, M. Fujiwara, O. Neitzke, T. Schröder, A. W. Schell, J. Wolters, J. Zheng, S. Mouradian, M. Almoktar, S. Takeuchi, D. Englund, and O. Benson, ACS Omega 2, 7194-7202 (2017) [2] “Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy“, B. Sontheimer, M. Braun, N. Nikolay, N. Sadzak, I. Aharonovich, and Oliver Benson, Phys. Rev B 96, 121202(R) (2017). [3] “Accurate placement of single nano particles on opaque conductive structures“, N. Nikolay, N. Sadzak, A. Dohms, B. Lubotzky, H. Abudayyeh, R. Rapaport, and O. Benson, Appl. Phys. Lett, accepted (2018); arXiv:1807.10605 [4] “Fine-tuning of whispering gallery modes in on-chip silica microdisk resonators within a full spectral range“, R. Henze, C. Pyrlik, A. Thies, J.M. Ward, A. Wicht, O. Benson, Appl. Phys. Lett. 102, 041104 (2013).
Collective light emission from many-body quantum systems is a cornerstone of quantum optics, yet its implementation in solid-state platforms operating under ambient conditions remains highly challenging. Large-bandgap van der Waals materials such as hexagonal boron nitride (hBN) host stable room-temperature single-photon emitters with narrow linewidths across a broad spectral range. However, cooperative radiative effects in this system have not been previously explored. Here we demonstrate collective emission from quantum-emitter ensembles in hBN layers when the emitters are nearly indistinguishable and positioned within a sub-wavelength proximity. Using confocal microscopy and a Hanbury Brown-Twiss (HBT) configuration, we identify both isolated emitters and ensembles activated by localized electron-beam irradiation. Time-resolved photoluminescence measurements reveal a superlinear intensity enhancement and a pronounced acceleration of the radiative decay in tightly confined ensembles, with lifetimes approaching the temporal resolution of our experimental system (about 500 ps), compared to approximately 1.85 ns for single emitters or large, spatially extended ensembles. Complementary second-order photon-correlation measurements exhibit sub-Poissonian antidip consistent with emission from a few indistinguishable emitters. The simultaneous observation of lifetime shortening and enhanced emission provides direct evidence of cooperative emission at room temperature, achieved without optical cavities or cryogenic cooling. These results establish optically active defect ensembles in hBN as a scalable solid-state platform for engineered collective quantum optics in two-dimensional materials, opening avenues toward ultrabright superradiant light sources and nonclassical photonic states for quantum technologies.