Volume 8, Issue 11 - Special Issue: Quantum Nanophotonics in Emerging Materials; Guest Editors: A. Alkauskas, L. C. Bassett; A. L. Exarhos; Kai-Mei Fu

Optically active point defects in wide-bandgap crystals are leading building blocks for quantum information technologies including quantum processors, repeaters, simulators, and sensors. Although defects and impurities are ubiquitous in all materials, select defect configurations in certain materials harbor coherent electronic and nuclear quantum states that can be optically and electronically addressed in solid-state devices, in some cases even at room temperature. Historically, the study of quantum point defects has been limited to a relatively small set of host materials and defect systems. In this article, we consider the potential for identifying defects in new materials, either to advance known applications in quantum science or to enable entirely new capabilities. We propose that, in principle, it should be possible to reverse the historical approach, which is partially based on accidental discovery, in order to design quantum defects with desired properties suitable for specific applications. We discuss the biggest obstacles on the road towards this goal, in particular those related to theoretical prediction, materials growth and processing, and experimental characterization.

Effective methods to generate colour centres in diamond and other wide band-gap materials are essential to the realisation of solid state quantum technologies based on such systems. Such methods have been the subject of intensive research effort in recent years. In this review, we bring together the various techniques used in the generation and positioning of colour centres in diamond: ion implantation, delta-doping, electron irradiation, laser writing and thermal annealing. We assess the roles and merits of each of these techniques in the formation of colour centres for different quantum technologies and consider future combinations of the techniques to meet the requirements of the most demanding applications.

The nitrogen-vacancy (NV) center in diamond is a solid-state defect qubit with favorable coherence time up to room temperature, which could be harnessed in several quantum-enhanced sensor and quantum communication applications, and has a potential in quantum simulation and computing. The quantum control largely depends on the intricate details about the electronic structure and states of the NV center, the radiative and nonradiative rates between these states, and the coupling of these states to external spins, electric, magnetic, and strain fields, and temperature. This review shows how first-principles calculations contributed to understanding the properties of the NV center and briefly discusses the issues to be solved toward the full ab initio description of solid-state defect qubits.

We provide an overview of the experimental techniques, measurement modalities, and diverse applications of the quantum diamond microscope (QDM). The QDM employs a dense layer of fluorescent nitrogen-vacancy (NV) color centers near the surface of a transparent diamond chip on which a sample of interest is placed. NV electronic spins are coherently probed with microwaves and optically initialized and read out to provide spatially resolved maps of local magnetic fields. NV fluorescence is measured simultaneously across the diamond surface, resulting in a wide-field, two-dimensional magnetic field image with adjustable spatial pixel size set by the parameters of the imaging system. NV measurement protocols are tailored for imaging of broadband and narrowband fields, from DC to GHz frequencies. Here we summarize the physical principles common to diverse implementations of the QDM and review example applications of the technology in geoscience, biology, and materials science.

The nitrogen-vacancy (NV) color center in diamond has rapidly emerged as an important solid-state system for quantum information processing. Whereas individual spin registers have been used to implement small-scale diamond quantum computing, the realization of a large-scale device requires the development of an on-chip quantum bus for transporting information between distant qubits. Here, we propose a method for coherent quantum transport of an electron and its spin state between distant NV centers. Transport is achieved by the implementation of spatial stimulated adiabatic Raman passage through the optical control of the NV center charge states and the confined conduction states of a diamond nanostructure. Our models show that, for two NV centers in a diamond nanowire, high-fidelity transport can be achieved over distances of order hundreds of nanometers in timescales of order hundreds of nanoseconds. Spatial adiabatic passage is therefore a promising option for realizing an on-chip spin quantum bus.

The nitrogen-vacancy (NV) center in diamond is a widely utilized system due to its useful quantum properties. Almost all research focuses on the negative charge state (NV − ) and comparatively little is understood about the neutral charge state (NV 0 ). This is surprising as the charge state often fluctuates between NV 0 and NV − during measurements. There are potentially under-utilized technical applications that could take advantage of NV 0 , either by improving the performance of NV 0 or utilizing NV − directly. However, the fine structure of NV 0 has not been observed. Here, we rectify this lack of knowledge by performing magnetic circular dichroism measurements that quantitatively determine the fine structure of NV 0 . The observed behavior is accurately described by spin-Hamiltonians in the ground and excited states with the ground state yielding a spin-orbit coupling of λ  = 2.24 ± 0.05 GHz and a orbital g -factor of 0.0186 ± 0.0005. The reasons why this fine structure has not been previously measured are discussed and strain-broadening is concluded to be the likely reason.

The ST1 center is a point defect in diamond with bright fluorescence and a mechanism for optical spin initialization and readout. The center has impressive potential for applications in diamond quantum computing as a quantum bus to a register of nuclear spins. This is because it has an exceptionally high readout contrast, and unlike the well-known nitrogen-vacancy center, it does not have a ground state electronic spin that decoheres the nuclear spins. However, its chemical structure is unknown, and there are large gaps in our understanding of its properties. We present the discovery of ST1 centers in natural diamond. Our experiments identify interesting power dependence of the center’s optical dynamics and reveal new electronic structure. We also present a theory of its electron-phonon interactions, which we combine with previous experiments, to shortlist likely candidates for its chemical structure.

Rare-earth dopants are arguably one of the most studied optical centers in solids, with applications spanning from laser optoelectronics, biosensing, lighting to displays. Nevertheless, harnessing rare-earth dopants’ extraordinary coherence properties for quantum information technologies is a relatively new endeavor, and has been rapidly advancing in recent years. Leveraging the state-of-the-art photonic technologies, on-chip rare-earth quantum devices functioning as quantum memories, single photon sources and transducers have emerged, often with potential performances unrivaled by other solid-state quantum technologies. These existing quantum devices, however, nearly exclusively rely on macroscopic bulk materials as substrates, which may limit future scalability and functionalities of such quantum systems. Thus, the development of new platforms beyond single crystal bulk materials has become an interesting approach. In this review article, we summarize the latest progress towards nanoscale, low-dimensional rare-earth doped materials for enabling next generation rare-earth quantum devices. Different platforms with a variety of synthesis methods are surveyed. Their key metrics measured to date are presented and compared. Special attention is placed on the connection between the topology of each platform to its target device applications. Lastly, an outlook for near term prospects of these platforms are given, with a hope to spur broader interests in rare-earth doped materials as a promising candidate for quantum information technologies.

Two-dimensional (2D) materials are being actively researched due to their exotic electronic and optical properties, including a layer-dependent bandgap, a strong exciton binding energy, and a direct optical access to electron valley index in momentum space. Recently, it was discovered that 2D materials with bandgaps could host quantum emitters with exceptional brightness, spectral tunability, and, in some cases, also spin properties. This review considers the recent progress in the experimental and theoretical understanding of these localized defect-like emitters in a variety of 2D materials as well as the future advantages and challenges on the path toward practical applications.

Control over individual point defects in solid-state systems is becoming increasingly important, not only for current semiconductor industries but also for next generation quantum information science and technologies. To realize the potential of these defects for scalable and high-performance quantum applications, precise placement of defects and defect clusters at the nanoscale is required, along with improved control over the nanoscale local environment to minimize decoherence. These requirements are met using scanned probe microscopy in silicon and III-V semiconductors, which suggests the extension to hosts for quantum point defects such as diamond, silicon carbide, and hexagonal boron nitride is feasible. Here we provide a perspective on the principal challenges toward this end, and new opportunities afforded by the integration of scanned probes with optical and magnetic resonance techniques.

In recent years, mono-layers and multi-layers of hexagonal boron nitride (hBN) have been demonstrated as host materials for localized atomic defects that can be used as emitters for ultra-bright, non-classical light. The origin of the emission, however, is still subject to debate. Based on measurements of photon statistics, lifetime and polarization on selected emitters, we find that these atomic defects do not act as pure single photon emitters. Our results strongly and consistently indicate that each zero phonon line of individual emitters comprises two independent electronic transitions. These results give new insights into the nature of the observed emission and hint at a double defect nature of emitters in multi-layer hBN.

Single-photon emitters (SPEs) in hexagonal boron nitride (hBN) are promising components for on-chip quantum information processing. Recently, large-area hBN films prepared by chemical vapor deposition (CVD) were found to host uniform, high densities of SPEs. However, the purity of these emitters has, to date, been low, hindering their applications in practical devices. In this work, we present two methods for post-growth processing of hBN, which significantly improve SPEs in hBN films that had been transferred from substrates used for CVD. The emitters exhibit high photon purities in excess of 90% and narrow linewidths of ~3 nm at room temperature. Our work lays a foundation for producing high-quality emitters in an ultra-compact two-dimensional material system and paves the way for deployment of hBN SPEs in scalable on-chip photonic and quantum devices.

The cooperative phenomena stemming from the radiation field-mediated coupling between individual quantum emitters are presently attracting broad interest for applications related to on-chip photonic quantum memories and long-range entanglement. Common to these applications is the generation of electro-magnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems wherein emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material (hexagonal boron nitride) to couple to a delocalized high-quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as single-photon sources at room temperature.