Temperature-Dependent Photophysics of Single NV Centers in Diamond.

We present a comprehensive study of the temperature- and magnetic-field-dependent photoluminescence (PL) of individual NV centers in diamond, spanning the temperature-range from cryogenic to ambient conditions. We directly observe the emergence of the NV's room-temperature effective excited-state structure and provide a clear explanation for a previously poorly understood broad quenching of NV PL at intermediate temperatures around 50 K, as well as the subsequent revival of NV PL. We develop a model based on two-phonon orbital averaging that quantitatively explains all of our findings, including the strong impact that strain has on the temperature dependence of the NV's PL. These results complete our understanding of orbital averaging in the NV excited state and have significant implications for the fundamental understanding of the NV center and its applications in quantum sensing.

Low-Temperature Photophysics of Single Nitrogen-Vacancy Centers in Diamond.

We investigate the magnetic field dependent photophysics of individual nitrogen-vacancy (NV) color centers in diamond under cryogenic conditions. At distinct magnetic fields, we observe significant reductions in the NV photoluminescence rate, which indicate a marked decrease in the optical readout efficiency of the NV's ground state spin. We assign these dips to excited state level anticrossings, which occur at magnetic fields that strongly depend on the effective, local strain environment of the NV center. Our results offer new insights into the structure of the NVs' excited states and a new tool for their effective characterization. Using this tool, we observe strong indications for strain-dependent variations of the NV's orbital g factor, obtain new insights into NV charge state dynamics, and draw important conclusions regarding the applicability of NV centers for low-temperature quantum sensing.

Probing Charge Dynamics in Diamond with an Individual Color Center.

Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV2-. These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.

First-Principles Identification of Single Photon Emitters Based on Carbon Clusters in Hexagonal Boron Nitride.

A recent study associates carbon with single photon emitters (SPEs) in hexagonal boron nitride (h-BN). This observation, together with the high mobility of carbon in h-BN, suggests the existence of SPEs based on carbon clusters. Here, by means of density functional theory calculations, we studied clusters of substitutional carbon atoms up to tetramers in h-BN. Two different conformations of neutral carbon trimers have zero-point line energies and shifts of the phonon sideband compatible with typical photoluminescence spectra. Moreover, some conformations of two small C clusters next to each other result in photoluminescence spectra similar to those found in the experiments. We also showed that vacancies are unable to reproduce the typical features of the phonon sideband observed in most measurements because of the large spectral weight of low-energy breathing modes, ubiquitous in such defects.

Functionalization of stable fluorescent nanodiamonds towards reliable detection of biomarkers for Alzheimer's disease.

BACKGROUND: Stable and non-toxic fluorescent markers are gaining attention in molecular diagnostics as powerful tools for enabling long and reliable biological studies. Such markers should not only have a long half-life under several assay conditions showing no photo bleaching or blinking but also, they must allow for their conjugation or functionalization as a crucial step for numerous applications such as cellular tracking, biomarker detection and drug delivery. RESULTS: We report the functionalization of stable fluorescent markers based on nanodiamonds (NDs) with a bifunctional peptide. This peptide is made of a cell penetrating peptide and a six amino acids long ß-sheet breaker peptide that is able to recognize amyloid ß (Aß) aggregates, a biomarker for the Alzheimer disease. Our results indicate that functionalized NDs (fNDs) are not cytotoxic and can be internalized by the cells. The fNDs allow ultrasensitive detection (at picomolar concentrations of NDs) of in vitro amyloid fibrils and amyloid aggregates in AD mice brains. CONCLUSIONS: The fluorescence of functionalized NDs is more stable than that of fluorescent markers commonly used to stain Aß aggregates such as Thioflavin T. These results pave the way for performing ultrasensitive and reliable detection of Aß aggregates involved in the pathogenesis of the Alzheimer disease.

Electronic structure of the silicon vacancy color center in diamond.

The negatively charged silicon vacancy (SiV) color center in diamond has recently proven its suitability for bright and stable single photon emission. However, its electronic structure so far has remained elusive. We here explore the electronic structure by exposing single SiV defects to a magnetic field where the Zeeman effect lifts the degeneracy of magnetic sublevels. The similar responses of single centers and a SiV ensemble in a low strain reference sample prove our ability to fabricate almost perfect single SiVs, revealing the true nature of the defect's electronic properties. We model the electronic states using a group-theoretical approach yielding a good agreement with the experimental observations. Furthermore, the model correctly predicts polarization measurements on single SiV centers and explains recently discovered spin selective excitation of SiV defects.

Collective enhancement in dissipative quantum batteries.

We study a quantum battery made out of N nonmutually interacting qubits coupled to a dissipative single electromagnetic field mode in a resonator. We quantify the charging energy, ergotropy, transfer rate, and power of the system, showing that collective enhancements are still present despite losses, and can even increase with dissipation. Moreover, we observe that a performance deterioration due to dissipation can be reduced by scaling up the battery size. This is useful for experimental realizations when controlling the quality of the resonator and the number of qubits are limiting factors.

Diffraction unlimited all-optical recording of electron spin resonances.

We show stimulated emission depletion microscopy to break the diffraction limit in the all-far-field-optical detection of magnetic fields and resonances. Electron spin resonances from single nitrogen-vacancy centers in diamond located at subdiffraction proximities are fully discerned. Since diffraction is overcome by disallowing the signaling state through an optical transition such as stimulated emission, the spin state remains unaffected and amenable to microwave manipulation. Stimulated emission depletion presents a universal scheme for superresolving spin resonances detectable by fluorescence.

Sensing Electrochemical Signals Using a Nitrogen-Vacancy Center in Diamond.

Chemical sensors with high sensitivity that can be used under extreme conditions and can be miniaturized are of high interest in science and industry. The nitrogen-vacancy (NV) center in diamond is an ideal candidate as a nanosensor due to the long coherence time of its electron spin and its optical accessibility. In this theoretical work, we propose the use of an NV center to detect electrochemical signals emerging from an electrolyte solution, thus obtaining a concentration sensor. For this purpose, we propose the use of the inhomogeneous dephasing rate of the electron spin of the NV center (1/T2★) as a signal. We show that for a range of mean ionic concentrations in the bulk of the electrolyte solution, the electric field fluctuations produced by the diffusional fluctuations in the local concentration of ions result in dephasing rates that can be inferred from free induction decay measurements. Moreover, we show that for a range of concentrations, the electric field generated at the position of the NV center can be used to estimate the concentration of ions.

High-fidelity spin and optical control of single silicon-vacancy centres in silicon carbide.

Scalable quantum networking requires quantum systems with quantum processing capabilities. Solid state spin systems with reliable spin-optical interfaces are a leading hardware in this regard. However, available systems suffer from large electron-phonon interaction or fast spin dephasing. Here, we demonstrate that the negatively charged silicon-vacancy centre in silicon carbide is immune to both drawbacks. Thanks to its 4A2 symmetry in ground and excited states, optical resonances are stable with near-Fourier-transform-limited linewidths, allowing exploitation of the spin selectivity of the optical transitions. In combination with millisecond-long spin coherence times originating from the high-purity crystal, we demonstrate high-fidelity optical initialization and coherent spin control, which we exploit to show coherent coupling to single nuclear spins with ∼1 kHz resolution. The summary of our findings makes this defect a prime candidate for realising memory-assisted quantum network applications using semiconductor-based spin-to-photon interfaces and coherently coupled nuclear spins.

A diamond nanowire single-photon source.

The development of a robust light source that emits one photon at a time will allow new technologies such as secure communication through quantum cryptography. Devices based on fluorescent dye molecules, quantum dots and carbon nanotubes have been demonstrated, but none has combined a high single-photon flux with stable, room-temperature operation. Luminescent centres in diamond have recently emerged as a stable alternative, and, in the case of nitrogen-vacancy centres, offer spin quantum bits with optical readout. However, these luminescent centres in bulk diamond crystals have the disadvantage of low photon out-coupling. Here, we demonstrate a single-photon source composed of a nitrogen-vacancy centre in a diamond nanowire, which produces ten times greater flux than bulk diamond devices, while using ten times less power. This result enables a new class of devices for photonic and quantum information processing based on nanostructured diamond, and could have a broader impact in nanoelectromechanical systems, sensing and scanning probe microscopy.