Single-photon emission from a high-purity hexagonal boron nitride crystal (Conference Presentation)

Optically active spin defects in wide-bandgap materials have many potential applications in quantum information and quantum sensing. Spin defects in two-dimensional layered van der Waals materials are just emerging to be investigated. Here we demonstrate that optically-addressable spin ensembles in hexagonal boron nitride (hBN) can be generated by femtosecond laser irradiation. We observe optically detected magnetic resonance (ODMR) of hBN spin defects created by laser irradiation. We show that the creation of spin defects in hBN is strongly affected by the pulse energy of the femtosecond laser. When the laser pulse number is less than a few thousand, the pulse number only affects the density of defects but not the type of defects. With proper laser parameters, spin defects can be generated with a high probability of success. Our work provides a convenient way to create spin defects in hBN by femtosecond laser writing, which shows promising prospects for quantum technologies.

Optically active defects in wide bandgap materials play a central role in several emerging applications in quantum information and sensing as they allow for manipulating and harvesting the internal degrees of freedom of single electrons with optical means. Interactions among defect states and with the surrounding environment represent a crucial feature for sensing but can severely hamper the coherence of the quantum states and prevent an efficient integration with photonic architectures due to unpredictable spectral instability. Understanding and controlling defect interactions would mitigate the effects of spectral instabilities and enable quantum applications based on long-range interactions. Here, we investigate the photoluminescence spectral dynamics of quantum emitters in defective hexagonal boron nitride (hBN), a material whose emission spectrum notoriously displays spectral wandering and diffusion, and we identify several optical transitions with discrete energy jumps. We associate the spectral jumps with the interplay amid competing recombination pathways available to the defect states in a process like donor-acceptor-pairs (DAP). The discrete spectral jumps observed in the emission spectrum of hBN arise from interactions between the harmonic states of nitrogen π orbitals of delocalized defects, and their energies can be ascribed to a DAP-like transition sequence. Our results allow mapping of the defect geometry in an hBN lattice, setting the basis for mitigating the effects of spectral jumping in this platform and paving the way toward using the long-range interaction of defect ensembles for quantum technology.

Solid-state sources of single-photon emitters are highly desired for scalable quantum photonic applications, such as quantum communication, optical quantum information processing, and metrology. In the past year, great strides have been made in the characterization of single defects in wide-bandgap materials, such as silicon carbide and diamond, as well as single molecules, quantum dots, and carbon nanotubes. More recently, single-photon emitters in layered van der Waals materials attracted tremendous attention, because the two-dimensional (2D) lattice allows for high photon extraction efficiency and easy integration into photonic circuits. In this review, we discuss recent advances in mastering single-photon emitters in 2D materials, electrical generation pathways, detuning, and resonator coupling towards use as quantum light sources. Finally, we discuss the remaining challenges and the outlooks for layered material-based quantum photonic sources.

The nitrogen-vacancy (NV) defect in diamond is an efficient quantum sensor of randomly fluctuating signals via relaxometry measurements. In particular, the longitudinal spin relaxation of the NV defect accelerates in the presence of magnetic noise with a spectral component at its electron spin resonance frequency. We look into this effect quantitatively by applying a calibrated and tunable magnetic noise on a single NV defect. We show that an increase of the longitudinal spin relaxation rate translates into a reduction of the photoluminescence (PL) signal emitted under continuous optical illumination, which can be explained using a simplified three-level model of the NV defect. This PL quenching mechanism offers a simple, all-optical method to detect magnetic noise sources at the nanoscale.

Characterization of deep defects in boron-doped CVD diamond films using transient photocapacitance method

The study of deep-level defects in semiconductors has always played a strategic role in the development of electronic and optoelectronic devices. Deep levels have a strong impact on many of the device properties, including efficiency, stability, and reliability, because they can drive several physical processes. Despite the advancements in crystal growth, wide- and ultrawide-bandgap semiconductors (such as gallium nitride and gallium oxide) are still strongly affected by the formation of defects that, in general, can act as carrier traps or generation-recombination centers (G-R). Conventional techniques used for deep-level analysis in silicon need to be adapted for identifying and characterizing defects in wide-bandgap materials. This topical review paper presents an overview of reviews of the theory of deep levels in semiconductors; in addition, we present a review and original results on the application, limits, and perspectives of two widely adopted common deep-level detection techniques, namely capacitance deep-level transient spectroscopy and deep-level optical spectroscopy, with specific focus on wide-bandgap semiconductors. Finally, the most common traps of GaN and β-Ga2O3 are reviewed.

We report progress in the development of tunable room temperature triggered single photon sources based on single nitrogen-vacancy (NV) centres in nanodiamond coupled to open access optical micro-cavities. The feeding of fluorescence from an NV centre into the cavity mode increases the spectral density of the emission and results in an output stream of triggered single photons with spectral line width of order 1 nm, tunable in the range 640 - 700 nm. We record single photon purities exceeding 96% and estimated device efficiencies up to 3%. We compare performance using plano-concave microcavities with radii of curvature from 25 μm to 4 μm and show that up to 17% of the total emission is fed into the TEM00 mode. Pulsed Hanbury-Brown Twiss (HBT) interferometry shows that an improvement in single photon purity is facilitated due to the increased spectral density.

For future quantum technologies and in particular for quantum architecture systems, one needs to consider scalability and reproducibility in order to be able to handle and add easily as many qubits of information as possible on a given platform. Quantum coherence and quantum information are fragile and thus requires the need for many qubits to be created, to interact and quantum information to be preserved. Currently there are either very good qubits in terms of fidelity but poor scalability or very good scalability but poor fidelity thus requiring more qubits to compensate. Most of the current platforms are in solid-state physics such as superconducting, dopants in silicon, quantum dots in III-V semiconductors or defects in diamond. The main interest for condensed matter systems is the fact that it is potentially scalable as integration is possible in the future, already demonstrated in the ‘classical’ semiconductor industry. Nevertheless, there are some true challenges in controlling and understanding the mechanisms of decoherence, losses and unwanted effects in these ‘dirty’ systems. As quantum technologies require ultimate control of quantum effects such as maintaining quantum coherence, quantum superposition and entanglement, it pushes towards deeper knowledge of underlying material and condensed matter physics. Photons are of particular interest as they are good carriers of quantum information and one aim is to explore a fully integrated photonic quantum circuit which would be a hybrid system made of stationary solid-state qubits (we will call them quantum emitters) coupled together via single photons travelling within a common optical bus that is photonics-ready for quantum communications within a network of quantum nodes. In this presentation, we will present our latest developments and results towards the integration of quantum emitters with photonic structures with nanosize features. In the first part, our platform is described which consists of glass and thus directly compatible with optical fibres. It is based on the technique of exchanged ions within the glass in order to create locally a particular confinement of the light. The next part will concern our latest results on two different quantum emitters. The first one is based on perovskite nanocristals that can be synthetised chemically and giving rise to quantum optics-type of emitters. The second one is based on the so-called silicon-vacancy defect centre in nanodiamonds. These emitters are produced by the high-pressure/high-temperature method and lead to promising results for quantum technologies. Finally, the last part will treat the nanophotonics approaches in order to couple efficiently these emitters with our platform.

This project will test the coupling of light emitted from silicon vacancy and nitrogen vacancy defects in diamond into additively manufactured photonic wire bonds toward integration into an "on-chip quantum photonics platform". These defects offer a room-temperature solid state solution for quantum information technologies but suffer from issues such as low activation rate and variable local environments. Photonic wire bonding will allow entanglement of pre-selected solid-state defects alleviating some of these issues and enable simplified integration with other photonic devices. These developments could prove to be key technologies to realize quantum secured networks for national security applications.

The exceptional spin coherence of nitrogen-vacancy centers in diamond motivates their function in emerging quantum technologies. Traditionally, the spin state of individual centers is measured optically and destructively. We demonstrate dispersive, single-spin coupling to light for both nondestructive spin measurement, through the Faraday effect, and coherent spin manipulation, through the optical Stark effect. These interactions can enable the coherent exchange of quantum information between single nitrogen-vacancy spins and light, facilitating coherent measurement, control, and entanglement that is scalable over large distances.

Mechanical systems can be influenced by a wide variety of small forces, ranging from gravitational to optical, electrical, and magnetic. When mechanical resonators are scaled down to nanometer-scale dimensions, these forces can be harnessed to enable coupling to individual quantum systems. We demonstrate that the coherent evolution of a single electronic spin associated with a nitrogen vacancy center in diamond can be coupled to the motion of a magnetized mechanical resonator. Coherent manipulation of the spin is used to sense driven and Brownian motion of the resonator under ambient conditions with a precision below 6 picometers. With future improvements, this technique could be used to detect mechanical zero-point fluctuations, realize strong spin-phonon coupling at a single quantum level, and implement quantum spin transducers.

We investigate spin and optical properties of individual nitrogen-vacancy\ncenters located within 1-10 nm from the diamond surface. We observe stable\ndefects with a characteristic optically detected magnetic resonance spectrum\ndown to lowest depth. We also find a small, but systematic spectral broadening\nfor defects shallower than about 2 nm. This broadening is consistent with the\npresence of a surface paramagnetic impurity layer [Tisler et al., ACS Nano 3,\n1959 (2009)] largely decoupled by motional averaging. The observation of stable\nand well-behaved defects very close to the surface is critical for single-spin\nsensors and devices requiring nanometer proximity to the target.\n

Nitrogen vacancy (NV) centers, optically active atomic defects in diamond, have attracted tremendous interest for quantum sensing, network, and computing applications due to their excellent quantum coherence and remarkable versatility in a real, ambient environment. One of the critical challenges to develop NV-based quantum operation platforms results from the difficulty in locally addressing the quantum spin states of individual NV spins in a scalable, energy-efficient manner. Here, we report electrical control of the coherent spin rotation rate of a single-spin qubit in NV-magnet based hybrid quantum systems. By utilizing electrically generated spin currents, we are able to achieve efficient tuning of magnetic damping and the amplitude of the dipole fields generated by a micrometer-sized resonant magnet, enabling electrical control of the Rabi oscillation frequency of NV spins. Our results highlight the potential of NV centers in designing functional hybrid solid-state systems for next-generation quantum-information technologies. The demonstrated coupling between the NV centers and the propagating spin waves harbored by a magnetic insulator further points to the possibility to establish macroscale entanglement between distant spin qubits.

Single-photon sources and their optical spin readout are at the core of applications in quantum communication, quantum computation, and quantum sensing. Their integration in photonic structures such as photonic crystals, microdisks, microring resonators, and nanopillars is essential for their deployment in quantum technologies. While there are currently only two material platforms (diamond and silicon carbide) with proven single-photon emission from the visible to infrared, a quantum spin–photon interface, and ancilla qubits, it is expected that other material platforms could emerge with similar characteristics in the near future. These two materials also naturally lead to monolithic integrated photonics as both are good photonic materials. While so far the verification of single-photon sources was based on discovery, assignment and then assessment and control of their quantum properties for applications, a better approach could be to identify applications and then search for the material that could address the requirements of the application in terms of quantum properties of the defects. This approach is quite difficult as it is based mostly on the reliability of modeling and predicting of color center properties in various materials, and their experimental verification is challenging. In this paper, we review some recent advances in an emerging material, low-dimensional (2D, 1D, 0D) hexagonal boron nitride (h-BN), which could lead to establishing such a platform. We highlight the recent achievements of the specific material for the expected applications in quantum technologies, indicating complementary outstanding properties compared to the other 3D bulk materials.

Quantum sensing with spin defects in diamond, such as the nitrogen vacancy (NV) center, enables the detection of various chemical species on the nanoscale. Molecules or ions with unpaired electronic spins are typically probed by their influence on the NV center's spin relaxation. Whereas it is well-known that paramagnetic ions reduce the NV center's relaxation time (T1), here we report on the opposite effect for diamagnetic ions. We demonstrate that millimolar concentrations of aqueous diamagnetic electrolyte solutions increase the T1 time of near-surface NV center ensembles compared to pure water. To elucidate the underlying mechanism of this surprising effect, single and double quantum NV experiments are performed, which indicate a reduction of magnetic and electric noise in the presence of diamagnetic electrolytes. In combination with ab initio simulations, we propose that a change in the interfacial band bending due to the formation of an electric double layer leads to a stabilization of fluctuating charges at the interface of an oxidized diamond. This work not only helps to understand noise sources in quantum systems but could also broaden the application space of quantum sensors toward electrolyte sensing in cell biology, neuroscience, and electrochemistry.