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The distinct spin, optical, and coherence characteristics of solid-state spin defects in semiconductors have positioned them as potential qubits for quantum technologies. Both bulk and two-dimensional materials, with varying structural properties, can serve as crystalline hosts for color centers. In this study, we conduct a comparative analysis of the spin–optical, electron–nuclear, and relaxation properties of nitrogen-bound vacancy defects using electron paramagnetic resonance (EPR) and electron–nuclear double resonance (ENDOR) techniques. We examine key parameters of the spin Hamiltonian for the nitrogen vacancy (NV−) center in 4H-SiC: D = 1.3 GHz, Azz = 1.1 MHz, and CQ = 2.53 MHz, as well as for the boron vacancy (VB−) in hBN: D = 3.6 GHz, Azz = 85 MHz, and CQ = 2.11 MHz, and their dependence on the material matrix. The spin–spin relaxation times T2 (NV− center: 50 µs and VB−: 15 µs) are influenced by the local nuclear environment and spin diffusion while Rabi oscillation damping times depend on crystal size and the spatial distribution of microwave excitation. The ENDOR absorption width varies significantly among color centers due to differences in crystal structures. These findings underscore the importance of selecting an appropriate material platform for developing quantum registers based on high-spin color centers in quantum information systems.

High-spin defects (color centers) in wide-gap semiconductors are considered as a basis for the implementation of quantum technologies due to the unique combination of their spin, optical, charge, and coherent properties. A silicon carbide (SiC) crystal can act as a matrix for a wide variety of optically active vacancy-type defects, which manifest themselves as single-photon sources or spin qubits. Among the defects, the nitrogen-vacancy centers (NV) are of particular importance. This paper is devoted to the application of the photoinduced electron paramagnetic resonance (EPR) and electron–nuclear double resonance (ENDOR) techniques at a high-frequency range (94 GHz) to obtain unique information about the nature and properties of NV defects in SiC crystal of the hexagonal 4H and 6H polytypes. Selective excitation by microwave and radio frequency pulses makes it possible to determine the microscopic structure of the color center, the zero-field splitting constant (D = 1.2–1.3 GHz), the phase coherence time (T2), and the values of hyperfine (≈1.1 MHz) and quadrupole (Cq ≈ 2.45 MHz) interactions and to define the isotropic (a = −1.2 MHz) and anisotropic (b = 10–20 kHz) contributions of the electron–nuclear interaction. The obtained data are essential for the implementation of the NV defects in SiC as quantum registers, enabling the optical initialization of the electron spin to establish spin–photon interfaces. Moreover, the combination of optical, microwave, and radio frequency resonant effects on spin centers within a SiC crystal shows the potential for employing pulse EPR and ENDOR sequences to implement protocols for quantum computing algorithms and gates.

Single-photon sources are important for integrated photonics and quantum technologies, and can be used in quantum key distribution, quantum computing, and sensing. Color centers in the solid state are a promising candidate for the development of the next generation of single-photon sources integrated in quantum photonics devices. They are point defects in a crystal lattice that absorb and emit light at given wavelengths and can emit single photons with high efficiency. The landscape of color centers has changed abruptly in recent years, with the identification of a wider set of color centers and the emergence of new solid-state platforms for room-temperature single-photon generation. This review discusses the emerging material platforms hosting single-photon-emitting color centers, with an emphasis on their potential for the development of integrated optical circuits for quantum photonics.

We report the development of multifunctional core/shell chemical vapor deposition diamond nanoparticles for the local photoinduced hyperthermia, thermometry, and fluorescent imaging. The diamond core heavily doped with boron is heated due to absorbed laser radiation and in turn heats the shell of a thin transparent diamond layer with embedded negatively charged SiV color centers emitting intense and narrowband zero-phonon lines with a temperature-dependent wavelength near 738 nm. The heating of the core/shell diamond nanoparticle is indicated by the temperature-induced spectral shift in the intensive zero-phonon line of the SiV color centers embedded in the diamond shell. The temperature of the core/shell diamond particles can be precisely manipulated by the power of the incident light. At laser power safe for biological systems, the photoinduced temperature of the core/shell diamond nanoparticles is high enough to be used for hyperthermia therapy and local nanothermometry, while the high zero-phonon line intensity of the SiV color centers allows for the fluorescent imaging of treated areas.

Lithium fluoride (LiF) film detectors for extreme ultraviolet radiation, soft and hard X-rays, based on the photoluminescence of radiation-induced electronic defects, have been proposed and are currently under further development and investigation. LiF film detectors are versatile and can be integrated in different experimental apparatus and imaging configurations. LiF can be grown in the form of polycrystalline thin films and it is compatible with several substrates. The radiation-induced color center (CCs) photoluminescence (PL) response can be enhanced through the appropriate choice of substrates and multilayer designs, and by tailoring the micro-structural properties of polycrystalline LiF films through the control of the growth conditions. In this work, we present the characterization, through fluorescence and Raman micro-spectroscopy, of LiF films, thermally evaporated on different substrates with thicknesses of up to 1 μm, irradiated with soft X-rays produced by a laser plasma source. The combination of these micro-spectroscopy techniques could represent an advanced method to investigate the role of the polycrystalline film structures in CC formation efficiency at the microscopic level, a fundamental aspect of the development of LiF film radiation-imaging detectors.

Lithium fluoride (LiF) crystals and thin films are utilized as radiation detectors for energy diagnostics of proton beams. This is achieved by analyzing the Bragg curves in LiF obtained by imaging the radiophotoluminescence of color centers created by protons. In LiF crystals, the Bragg peak depth increases superlinearly with the particle energy. A previous study has shown that, when 35 MeV protons impinge at grazing incidence onto LiF films deposited on Si(100) substrates, the Bragg peak in the films is located at the depth where it would be found in Si rather than in LiF due to multiple Coulomb scattering. In this paper, Monte Carlo simulations of proton irradiations in the 1–8 MeV energy range are performed and compared to experimental Bragg curves in optically transparent LiF films on Si(100) substrates. Our study focuses on this energy range because, as energy increases, the Bragg peak gradually shifts from the depth in LiF to that in Si. The impact of grazing incidence angle, LiF packing density, and film thickness on shaping the Bragg curve in the film is examined. At energies higher than 8 MeV, all these quantities must be considered, although the effect of packing density plays a minor role.

The physical properties of diamond crystals, such as color or electrical conductivity, can be controlled via impurities. In particular, when doped with nitrogen, optically active nitrogen-vacancy centers (NV), can be induced. The center is an outstanding quantum spin system that enables, under ambient conditions, optical initialization, readout, and coherent microwave control with applications in sensing and quantum information. Under optical and radio frequency excitation, the Zeeman splitting of the degenerate states allows the quantitative measurement of external magnetic fields with high sensitivity. This study provides a pedagogical introduction to the properties of the NV centers as well as a step-by-step process to develop and test a simple magnetic quantum sensor based on color centers with significant potential for the development of highly compact multisensor systems.

The gray-colored oxygen-deficient TiO2–δ(B) nanobelts have been synthesized through a combination of the hydrothermal method followed by an ion exchange process and vacuum annealing. Electron paramagnetic resonance reveals an existence of F-centers in the form of electron-trapped oxygen vacancies within the anionic sublattice of the gray bronze TiO2 that induces its colouration. The diffuse reflectance spectroscopy showed that the formation of oxygen vacancies into TiO2(B) significantly increases its absorption intensity in both visible and near infrared ranges. The band gap of TiO2(B) with anionic defects is equal to 3.03 eV (against 3.24 eV for white TiO2(B) treated in air). Room temperature ferromagnetism associated with the defects was detected in gray TiO2–δ(B), thus indicating it belongs it to the class of dilute magnetic oxide semiconductors. It was found that in the low-temperature range (4 K), the magnetic properties of vacuum annealed TiO2(B) do not differ from those for TiO2(B) treated in air. We hope that the findings are defined here make a contribution to further progress in fabrication and manufacturing of defective TiO2-based nanomaterials for catalysis, magnetic applications, batteries, etc.

Short-pulse ion beams have been developed in recent years and now enable applications in materials science. A tunable flux of selected ions delivered in pulses of a few nanoseconds can affect the balance of defect formation and dynamic annealing in materials. We report results from color center formation in silicon with pulses of 900 keV protons. G-centers in silicon are near-infrared photon emitters with emerging applications as single-photon sources and for spin-photon qubit integration. G-centers consist of a pair of substitutional carbon atoms and one silicon interstitial atom and are often formed by carbon ion implantation and thermal annealing. Here, we report on G-center formation with proton pulses in silicon samples that already contained carbon, without carbon ion implantation or thermal annealing. The number of G-centers formed per proton increased when we increased the pulse intensity from 6.9 × 109 to 7.9 × 1010 protons/cm2/pulse, demonstrating a flux effect on G-center formation efficiency. We observe a G-center ensemble linewidth of 0.1 nm (full width half maximum), narrower than previously reported. Pulsed ion beams can extend the parameter range available for fundamental studies of radiation-induced defects and the formation of color centers for spin-photon qubit applications.

Color centers in silicon carbide have recently emerged as one of the most promising emitters for bright single-photon emitting diodes (SPEDs). It has been shown that, at room temperature, they can emit more than 109 photons per second under electrical excitation. However, the spectral emission properties of color centers in SiC at room temperature are far from ideal. The spectral properties could be significantly improved by decreasing the operating temperature. However, the densities of free charge carriers in SiC rapidly decrease as temperature decreases, which reduces the efficiency of electrical excitation of color centers by many orders of magnitude. Here, we study for the first time the temperature characteristics of SPEDs based on color centers in 4H-SiC. Using a rigorous numerical approach, we demonstrate that although the single-photon electroluminescence rate does rapidly decrease as temperature decreases, it is possible to increase the SPED brightness to 107 photons/s at 100 K using the recently predicted effect of hole superinjection in homojunction p-i-n diodes. This gives the possibility to achieve high brightness and good spectral properties at the same time, which paves the way toward novel quantum photonics applications of electrically driven color centers in silicon carbide.

The negatively charged germanium-vacancy GeV− color centers in diamond nanocrystals are solid-state photon emitters suited for quantum information technologies, bio-sensing, and labeling applications. Due to the small Huang–Rhys factor, the GeV−-center zero-phonon line emission is expected to be very intensive and spectrally narrow. However, structural defects and the inhomogeneous distribution of local strains in the nanodiamonds result in the essential broadening of the ZPL. Therefore, clarification and elimination of the reasons for the broadening of the GeV− center ZPL is an important problem. We report on the effect of reactive ion etching in oxygen plasma on the structure and luminescence properties of nanodiamonds grown by hot filament chemical vapor deposition. Emission of GeV− color centers ensembles at about 602 nm in as-grown and etched nanodiamonds is probed using micro-photoluminescence and micro-Raman spectroscopy at room and liquid nitrogen temperature. We show that the etching removes the nanodiamond surface sp2-induced defects resulting in a reduction in the broad luminescence background and a narrowing of the diamond Raman band. The zero-phonon luminescence band of the ensemble of the GeV− centers is a superposition of narrow lines originated most likely from the GeV− center sub-ensembles under different uniaxial local strain conditions.

Radiation-induced color centers locally produced in lithium fluoride (LiF) are successfully used for radiation detectors. LiF detectors for extreme ultraviolet radiation, soft and hard X-rays, based on photoluminescence from aggregate electronic defects, are currently under development for imaging applications with laboratory radiation sources, as well as large-scale facilities. Among the peculiarities of LiF-based detectors, noteworthy ones are their very high intrinsic spatial resolution across a large field of view, wide dynamic range, and versatility. LiF crystals irradiated with a monochromatic 8 keV X-ray beam at KIT synchrotron light source (Karlsruhe, Germany) and with the broadband white beam spectrum of the synchrotron bending magnet have been investigated by optical spectroscopy, laser scanning confocal microscopy in fluorescence mode, and confocal Raman micro-spectroscopy. The 3D reconstruction of the distributions of the color centers induced by the X-rays has been performed with both confocal techniques. The combination of the LiF crystal capability to register volumetric X-ray mapping with the optical sectioning operations of the confocal techniques has allowed performing 3D reconstructions of the X-ray colored volumes and it could provide advanced tools for 3D X-ray detection.

Color centers in silicon carbide are relevant for applications in quantum technologies as they can produce single photon sources or can be used as spin qubits and in quantum sensing applications. Here, we have applied femtosecond laser writing in silicon carbide and gallium nitride to generate vacancy-related color centers, giving rise to photoluminescence from the visible to the infrared. Using a 515 nm wavelength 230 fs pulsed laser, we produce large arrays of silicon vacancy defects in silicon carbide with a high localization within the confocal diffraction limit of 500 nm and with minimal material damage. The number of color centers formed exhibited power-law scaling with the laser fabrication energy indicating that the color centers are created by photoinduced ionization. This work highlights the simplicity and flexibility of laser fabrication of color center arrays in relevant materials for quantum applications.

This contribution presents a personal account of the influence Karl Alex Müller had on the early stages of my career and the scientific questions about which we exchanged our views over the years. While both our research branched into a variety of topics, the common experimental technique, Electron Paramagnetic Resonance, and the Jahn-Teller effect led to fruitful exchanges of ideas on these matters in semiconducting, metallic and ionic crystals.

Many promising applications of single crystal diamond and its color centers as sensor platform and in photonics require free-standing membranes with a thickness ranging from several micrometers to the few 100 nm range. In this work, we present an approach to conveniently fabricate such thin membranes with up to about one millimeter in size. We use commercially available diamond plates (thickness 50 μ m) in an inductively coupled reactive ion etching process which is based on argon, oxygen and SF 6 . We thus avoid using toxic, corrosive feed gases and add an alternative to previously presented recipes involving chlorine-based etching steps. Our membranes are smooth (RMS roughness

This special issue is intended to serve as a multidisciplinary forum covering broad aspects of the science, technology, and application of synthetic and natural diamonds. This special issue contains 12 papers, which highlight recent investigations and developments in diamond research related to the diverse problems of natural diamond genesis, diamond synthesis and growth using CVD and HPHT techniques, and the use of diamond in both traditional applications, such as mechanical machining of materials, and the new recently emerged areas, such as quantum technologies. The results presented in the contributions collected in this special issue clearly demonstrate that diamond occupies a very special place in modern science and technology. After decades of research, this structurally very simple material still poses many intriguing scientific questions and technological challenges. It seems undoubted that diamond will remain the center of attraction for many researchers for many years to come.