Precise Characterization of a Waveguide Fiber Interface in Silicon Carbide.

Spin-active optical emitters in silicon carbide are excellent candidates toward the development of scalable quantum technologies. However, efficient photon collection is challenged by undirected emission patterns from optical dipoles, as well as low total internal reflection angles due to the high refractive index of silicon carbide. Based on recent advances with emitters in silicon carbide waveguides, we now demonstrate a comprehensive study of nanophotonic waveguide-to-fiber interfaces in silicon carbide. We find that across a large range of fabrication parameters, our experimental collection efficiencies remain above 90%. Further, by integrating silicon vacancy color centers into these waveguides, we demonstrate an overall photon count rate of 181 kilo-counts per second, which is an order of magnitude higher compared to standard setups. We also quantify the shift of the ground state spin states due to strain fields, which can be introduced by waveguide fabrication techniques. Finally, we show coherent electron spin manipulation with waveguide-integrated emitters with state-of-the-art coherence times of T 2 ∼ 42 µs. The robustness of our methods is very promising for quantum networks based on multiple orchestrated emitters.

Near-zero-field microwave-free magnetometry with nitrogen-vacancy centers in nanodiamonds.

We study the fluorescence of nanodiamond ensembles as a function of static external magnetic field and observe characteristic dip features close to the zero field with potential for magnetometry applications. We analyze the dependence of the feature's width and the contrast of the feature on the size of the diamond (in the range 30 nm-3000 nm) and on the strength of a bias magnetic field applied transversely to the field being scanned. We also perform optically detected magnetic resonance (ODMR) measurements to quantify the strain splitting of the zero-field ODMR resonance across various nanodiamond sizes and compare it with the width and contrast measurements of the zero-field fluorescence features for both nanodiamonds and bulk samples. The observed properties provide compelling evidence of cross-relaxation effects in the NV system occurring close to zero magnetic fields. Finally, the potential of this technique for use in practical magnetometry is discussed.

Terahertz emission from diamond nitrogen-vacancy centers.

Coherent light sources emitting in the terahertz range are highly sought after for fundamental research and applications. Terahertz lasers rely on achieving population inversion. We demonstrate the generation of terahertz radiation using nitrogen-vacancy centers in a diamond single crystal. Population inversion is achieved through the Zeeman splitting of the S = 1 state in 15 tesla, resulting in a splitting of 0.42 terahertz, where the middle Sz = 0 sublevel is selectively pumped by visible light. To detect the terahertz radiation, we use a phase-sensitive terahertz setup, optimized for electron spin resonance (ESR) measurements. We determine the spin-lattice relaxation time up to 15 tesla using the light-induced ESR measurement, which shows the dominance of phonon-mediated relaxation and the high efficacy of the population inversion. The terahertz radiation is tunable by the magnetic field, thus these findings may lead to the next generation of tunable coherent terahertz sources.

Diamond surface functionalization via visible light-driven C-H activation for nanoscale quantum sensing.

Nitrogen-vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV-based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution-phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single-crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single-crystal surfaces, and solution-phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C-H bonds on single-crystal diamond surfaces under ambient conditions using visible light, forming C-F, C-Cl, C-S, and C-N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to the state of the art. As a proof-of-principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface-bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single-molecule spectroscopy.

Resonant Versus Nonresonant Spin Readout of a Nitrogen-Vacancy Center in Diamond under Cryogenic Conditions.

The last decade has seen an explosive growth in the use of color centers for metrology applications, the paradigm example arguably being the nitrogen-vacancy (NV) center in diamond. Here, we focus on the regime of cryogenic temperatures and examine the impact of spin-selective, narrow-band laser excitation on NV readout. Specifically, we demonstrate a more than fourfold improvement in sensitivity compared to that possible with nonresonant (green) illumination, largely due to a boost in readout contrast and integrated photon count. We also leverage nuclear spin relaxation under resonant excitation to polarize the ^{14}N host, which we then prove beneficial for spin magnetometry. These results open opportunities in the application of NV sensing to the investigation of condensed matter systems, particularly those exhibiting superconducting, magnetic, or topological phases selectively present at low temperatures.

Formation of Paramagnetic Defects in the Synthesis of Silicon Carbide.

Silicon carbide (SiC) is a very promising platform for quantum information processing, as it can host room temperature solid state defect quantum bits. These room temperature quantum bits are realized by paramagnetic silicon vacancy and divacancy defects in SiC that are typically introduced by irradiation techniques. However, irradiation techniques often introduce unwanted defects near the target quantum bit defects that can be detrimental for the operation of quantum bits. Here, we demonstrate that by adding aluminum precursor to the silicon and carbon sources, quantum bit defects are created in the synthesis of SiC without any post treatments. We optimized the synthesis parameters to maximize the paramagnetic defect concentrations-including already established defect quantum bits-monitored by electron spin resonance spectroscopy.

Amino-Termination of Silicon Carbide Nanoparticles.

Silicon carbide nanoparticles (SiC NPs) are promising inorganic molecular-sized fluorescent biomarkers. It is imperative to develop methods to functionalize SiC NPs for certain biological applications. One possible route is to form amino groups on the surface, which can be readily used to attach target biomolecules. Here, we report direct amino-termination of aqueous SiC NPs. We demonstrate the applicability of the amino-terminated SiC NPs by attaching bovine serum albumin as a model for functionalization. We monitor the optical properties of the SiC NPs in this process and find that the fluorescence intensity is very sensitive to surface termination. Our finding may have implications for a few nanometers sized SiC NPs containing paramagnetic color centers with optically read electron spins.

Investigation of oxygen-vacancy complexes in diamond by means ofab initiocalculations.

Point defects in diamond may act as quantum bits. Recently, oxygen-vacancy related defects have been proposed to the origin of the so-called ST1 color center in diamond that can realize a long-living solid-state quantum memory. Motivated by this proposal we systematically investigate oxygen-vacancy complexes in diamond by means of first principles density functional theory calculations. We find that all the considered oxygen-vacancy defects have a high-spin ground state in their neutral charge state, which disregards them as an origin for the ST1 color center. We identify a high-spin metastable oxygen-vacancy complex and characterize their magneto-optical properties for identification in future experiments.

Coherent control of an ultrabright single spin in hexagonal boron nitride at room temperature.

Hexagonal boron nitride (hBN) is a remarkable two-dimensional (2D) material that hosts solid-state spins and has great potential to be used in quantum information applications, including quantum networks. However, in this application, both the optical and spin properties are crucial for single spins but have not yet been discovered simultaneously for hBN spins. Here, we realize an efficient method for arraying and isolating the single defects of hBN and use this method to discover a new spin defect with a high probability of 85%. This single defect exhibits outstanding optical properties and an optically controllable spin, as indicated by the observed significant Rabi oscillation and Hahn echo experiments at room temperature. First principles calculations indicate that complexes of carbon and oxygen dopants may be the origin of the single spin defects. This provides a possibility for further addressing spins that can be optically controlled.

The Role of Electrolytes in the Relaxation of Near-Surface Spin Defects in Diamond.

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.

Controlled Surface Modification to Revive Shallow NV- Centers.

Near-surface negatively charged nitrogen vacancy (NV) centers hold excellent promise for nanoscale magnetic imaging and quantum sensing. However, they often experience charge-state instabilities, leading to strongly reduced fluorescence and NV coherence time, which negatively impact magnetic imaging sensitivity. This occurs even more severely at 4 K and ultrahigh vacuum (UHV, p = 2 × 10-10 mbar). We demonstrate that in situ adsorption of H2O on the diamond surface allows the partial recovery of the shallow NV sensors. Combining these with band-bending calculations, we conclude that controlled surface treatments are essential for implementing NV-based quantum sensing protocols under cryogenic UHV conditions.

A Telecom O-Band Emitter in Diamond.

Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communication and unfavorable for imaging in biological tissues. Here, we report the experimental observation of a new color center that emits in the telecom O-band, which we observe in silicon-doped bulk single crystal diamonds and microdiamonds. Combining absorption and photoluminescence measurements, we identify a zero-phonon line at 1221 nm and phonon replicas separated by 42 meV. Using transient absorption spectroscopy, we measure an excited state lifetime of around 270 ps and observe a long-lived baseline that may arise from intersystem crossing to another spin manifold.

The kinetics of carbon pair formation in silicon prohibits reaching thermal equilibrium.

Thermal equilibrium is reached when the system assumes its lowest energy. This can be hindered by kinetic reasons; however, it is a general assumption that the ground state can be eventually reached. Here, we show that this is not always necessarily the case. Carbon pairs in silicon have at least three different configurations, one of them (B-configuration) is the G photoluminescence centre. Experiments revealed a bistable nature with the A-configuration. Electronic structure calculations predicted that the C-configuration is the real ground state; however, no experimental evidence was found for its existence. Our calculations show that the formation of the A- and B-configurations is strongly favoured over the most stable C-configuration which cannot be realized in a detectable amount before the pair dissociates. Our results demonstrate that automatized search for complex defects consisting of only the thermodynamically most stable configurations may overlook key candidates for quantum technology applications.

Identification of an Oxygen Defect in Hexagonal Boron Nitride.

Paramagnetic fluorescent defects in two-dimensional hexagonal boron nitride (hBN) are promising building blocks for quantum information processing. Although numerous defect-related single-photon sources and a few quantum bits have been found, except for the boron vacancy, their identification is still elusive. Here, we demonstrate that the comparison of experimental and first-principles simulated electron paramagnetic resonance (EPR) spectra is a powerful tool for defect identification in hBN, and first-principles modeling is inevitable in this process as a result of the dense nuclear spin environment of hBN. In particular, a recently observed EPR center is associated with the negatively charged oxygen vacancy complex by means of the many-body perturbation theory method on top of hybrid density functional calculations. To our surprise, the negatively charged oxygen vacancy complex produces a coherent emission around 2 eV with a well-reproducing previously recorded photoluminescence spectrum of some quantum emitters, according to our calculations.

Coherent dynamics of multi-spin V[Formula: see text] center in hexagonal boron nitride.

Hexagonal boron nitride (hBN) has recently been demonstrated to contain optically polarized and detected electron spins that can be utilized for implementing qubits and quantum sensors in nanolayered-devices. Understanding the coherent dynamics of microwave driven spins in hBN is of crucial importance for advancing these emerging new technologies. Here, we demonstrate and study the Rabi oscillation and related phenomena of a negatively charged boron vacancy (V[Formula: see text]) spin ensemble in hBN. We report on different dynamics of the V[Formula: see text] spins at weak and strong magnetic fields. In the former case the defect behaves like a single electron spin system, while in the latter case it behaves like a multi-spin system exhibiting multiple-frequency dynamical oscillation as beat in the Ramsey fringes. We also carry out theoretical simulations for the spin dynamics of V[Formula: see text] and reveal that the nuclear spins can be driven via the strong electron nuclear coupling existing in V[Formula: see text] center, which can be modulated by the magnetic field and microwave field.

Room-temperature coherent manipulation of single-spin qubits in silicon carbide with a high readout contrast.

Spin defects in silicon carbide (SiC) with mature wafer-scale fabrication and micro/nano-processing technologies have recently drawn considerable attention. Although room-temperature single-spin manipulation of colour centres in SiC has been demonstrated, the typically detected contrast is less than 2[Formula: see text], and the photon count rate is also low. Here, we present the coherent manipulation of single divacancy spins in 4H-SiC with a high readout contrast ([Formula: see text]) and a high photon count rate (150 kilo counts per second) under ambient conditions, which are competitive with the nitrogen-vacancy centres in diamond. Coupling between a single defect spin and a nearby nuclear spin is also observed. We further provide a theoretical explanation for the high readout contrast by analysing the defect levels and decay paths. Since the high readout contrast is of utmost importance in many applications of quantum technologies, this work might open a new territory for SiC-based quantum devices with many advanced properties of the host material.

Ultraviolet Quantum Emitters in Hexagonal Boron Nitride from Carbon Clusters.

Ultraviolet (UV) quantum emitters in hexagonal boron nitride (hBN) have generated considerable interest due to their outstanding optical response. Recent experiments have identified a carbon impurity as a possible source of UV single-photon emission. Here, on the basis of first-principles calculations, we systematically evaluate the ability of substitutional carbon defects to develop the UV color centers in hBN. Of 17 defect configurations under consideration, we particularly emphasize the carbon ring defect (6C), for which the calculated zero-phonon line agrees well the experimental 4.1 eV emission signal. We also compare the optical properties of 6C with those of other relevant defects, thereby outlining the key differences in the emission mechanism. Our findings provide new insights into the strong response of this color center to external perturbations and pave the way to a robust identification of the particular carbon substitutional defects by spectroscopic methods.

Carbon defect qubit in two-dimensional WS2.

Identifying and fabricating defect qubits in two-dimensional semiconductors are of great interest in exploring candidates for quantum information and sensing applications. A milestone has been recently achieved by demonstrating that single defect, a carbon atom substituting sulphur atom in single layer tungsten disulphide, can be engineered on demand at atomic size level precision, which holds a promise for a scalable and addressable unit. It is an immediate quest to reveal its potential as a qubit. To this end, we determine its electronic structure and optical properties from first principles. We identify the fingerprint of the neutral charge state of the defect in the scanning tunnelling spectrum. In the neutral defect, the giant spin-orbit coupling mixes the singlet and triplet excited states with resulting in phosphorescence at the telecom band that can be used to read out the spin state, and coherent driving with microwave excitation is also viable. Our results establish a scalable qubit in a two-dimensional material with spin-photon interface at the telecom wavelength region.

Identification of a Telecom Wavelength Single Photon Emitter in Silicon.

We identify the exact microscopic structure of the G photoluminescence center in silicon by first-principles calculations with including a self-consistent many-body perturbation method, which is a telecommunication wavelength single photon source. The defect constitutes of C_{s}C_{i} carbon impurities in its C_{s}─Si_{i}─C_{s} configuration in the neutral charge state, where s and i stand for the respective substitutional and interstitial positions in the Si lattice. We reveal that the observed fine structure of its optical signals originates from the athermal rotational reorientation of the defect. We attribute the monoclinic symmetry reported in optically detected magnetic resonance measurements to the reduced tunneling rate at very low temperatures. We discuss the thermally activated motional averaging of the defect properties and the nature of the qubit state.