Silicon-vacancy Centers Research Articles

Ultrasensitive All-Optical Thermometry Using Nanodiamonds with a High Concentration of Silicon-Vacancy Centers and Multiparametric Data Analysis

Nanoscale thermometry is paramount to study primary processes of heat transfer in solids and is a subject of hot debate in cell biology. Here we report ultrafast temperature sensing using all-optical thermometry, exploiting synthetic nanodiamonds with silicon-vacancy (SiV) centers embedded at a high concentration. Using multiparametric analysis of photoluminescence (PL) of these centers, we have experimentally achieved an intrinsic noise floor of about 13 mK Hz , which is a 1000-fold increase in the readout speed in comparison to the current record values demonstrated with all-optical methods of comparable spatial-resolution and precision. Our thermometers are smaller than 250 nm across but can detect a 0.4 °C change of temperature in a measurement taking only 0.001 s. The exceptional sensitivity and simplicity of these thermometers enable a wide range of applications such as temperature monitoring and mapping within intracellular regions and in state-of-the-art solid-state electronic nanodevices.

Initialization and Readout of Nuclear Spins via a Negatively Charged Silicon-Vacancy Center in Diamond.

In this Letter, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This Letter paves the way toward realization of building blocks of quantum hardware with an efficient spin-photon interface based on the SiV color center coupled to a long lasting nuclear memory.

Spin polarization through intersystem crossing in the silicon vacancy of silicon carbide

Silicon carbide (SiC)-based defects are promising for quantum communications, quantum information processing, and for the next generation of quantum sensors, as they feature long coherence times, frequencies near the telecom, and optical and microwave transitions. For such applications, the efficient initialization of the spin state is necessary. We develop a theoretical description of the spin polarization process by using the intersystem crossing of the silicon vacancy defect, which is enabled by a combination of optical driving, spin-orbit coupling, and interaction with vibrational modes. By using distinct optical drives, we analyze two spin polarization channels. Interestingly, we find that different spin projections of the ground state manifold can be polarized. This work helps to understand initialization and readout of the silicon vacancy and explains some existing experiments with the silicon vacancy center in SiC.

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.

Diamond photonics platform based on silicon vacancy centers in a single-crystal diamond membrane and a fiber cavity

We realize a potential platform for an efficient spin-photon interface, namely negatively-charged silicon-vacancy centers in a diamond membrane coupled to the mode of a fully-tunable, fiber-based, optical resonator. We demonstrate that introducing the thin ($\sim 200 \, \text{nm}$), single crystal diamond membrane into the mode of the resonator does not change the cavity properties, which is one of the crucial points for an efficient spin-photon interface. In particular, we observe constantly high Finesse values of up to $3000$ and a linear dispersion in the presence of the membrane. We observe cavity-coupled fluorescence froman ensemble of SiV$^{-}$ centers with an enhancement factor of $\sim 1.9$. Furthermore from our investigations we extract the ensemble absorption and extrapolate an absorption cross section of $(2.9 \, \pm \, 2) \, \cdot \, 10^{-12} \, \text{cm}^{2}$ for a single SiV$^{-}$ center, much higher than previously reported.

Electronic structure of the neutral silicon-vacancy center in diamond

The neutrally-charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency, broadband optical spin polarization with long spin lifetimes (T2 ~ 1 ms at 4 K) and up to 90% of optical emission into its 946 nm zero-phonon line. However, the electronic structure of SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u state is incorrect, and identify instead a coupled 3Eu - 3A2u system, the lower state of which has forbidden optical emission at zero stress and so efficiently decreases the total emission of the defect: we propose a solution employing finite strain to form the basis of a spin-photon interface. Isotopic enrichment definitively assigns the 976 nm transition associated with the defect to a local mode of the silicon atom.

Electronic structures of two-dimensional hydrogenated bilayer diamond films with Si dopant and Si-V center

Abstract The structural, electronic and optical properties of two-dimensional hydrogen-terminated bilayer diamond films (2D-HBDF) with silicon (Si) dopant and silicon-vacancy (Si-V) center are investigated by first-principles calculations. The two positions of substitutional Si are energetically favorable with similar band structures compared to the pristine 2D-HBDF. For Si-V center, the flat intermediate bands originated from the complex impurities appear in band gap. Especially, the ground state of paramagnetic or nonmagnetic for the case of Si-V is dependent on the distributions of Si dopant and vacancy. The calculated optical absorptions with relating to Si-V center show a high intensity in the visible light region. It reveals that the introducing vacancy (substituted Si) and their positions play an important role in modulating the electronic and optical properties of 2D-HBDF, which are helpful to construct novel low-dimensional diamond-based optoelectronic devices applied in extreme environments.

Laser Writing of Scalable Single Color Centers in Silicon Carbide.

Single photon emitters in silicon carbide (SiC) are attracting attention as quantum photonic systems ( Awschalom et al. Nat. Photonics 2018 , 12 , 516 - 527 ; Atatüre et al. Nat. Rev. Mater. 2018 , 3 , 38 - 51 ). However, to achieve scalable devices, it is essential to generate single photon emitters at desired locations on demand. Here we report the controlled creation of single silicon vacancy (VSi) centers in 4H-SiC using laser writing without any postannealing process. Due to the aberration correction in the writing apparatus and the nonannealing process, we generate single VSi centers with yields up to 30%, located within about 80 nm of the desired position in the transverse plane. We also investigated the photophysics of the laser writing VSi centers and concluded that there are about 16 photons involved in the laser writing VSi center process. Our results represent a powerful tool in the fabrication of single VSi centers in SiC for quantum technologies and provide further insights into laser writing defects in dielectric materials.

Formation of GeV, SiV, and NV Color Centers in Single Crystal Diamond Needles Grown by Chemical Vapor Deposition

Herein the color centers formation in diamond crystallites of pyramidal shape grown by chemical vapor deposition (CVD) is described. The individual crystallites are extracted from polycrystalline films grown on silicon substrates. The silicon‐vacancy (SiV), germanium‐vacancy (GeV), and nitrogen‐vacancy (NV) centers are created by introducing corresponding precursors from substrate material, gaseous nitrogen, and thermally evaporated germanium added during CVD. Some amount of NV centers detected in all types of the diamond crystallites is assigned to uncontrollable presence of nitrogen in the CVD reactor. The low temperature photoluminescence spectra indicate presence of ensembles of SiV centers in diamond structure. The SiV centers are concentrated predominantly at apexes of the diamond crystallites located at substrate surface. Intense growth of CN radicals in plasma‐activated gas environment during CVD process is detected after nitrogen gas addition. The crystallites obtained with the nitrogen addition demonstrate significant variation of their pyramid angle. The photoluminescence spectra of crystallites grown with nitrogen addition demonstrate increase of both negatively and neutrally charged states of NV color center. The GeV centers are created via thermal evaporation of pure Ge during CVD growth. The photoluminescence spectra of the crystallites grown with Ge addition demonstrate presence of GeV color centers ensemble.

Coherent Control and Wave Mixing in an Ensemble of Silicon-Vacancy Centers in Diamond.

Strong light-matter interactions are critical for quantum technologies based on light, such as memories or nonlinear interactions. Solid state materials will be particularly important for such applications due to the relative ease of fabrication of components. Silicon vacancy centers (SiV^{-}) in diamond feature especially narrow inhomogeneous spectral lines, which are rare in solid materials. Here, we demonstrate resonant coherent manipulation, stimulated Raman adiabatic passage, and strong light-matter interaction via the four-wave mixing of a weak signal field in an ensemble of SiV^{-} centers.

Toward wafer-scale diamond nano- and quantum technologies

We investigate native nitrogen vacancy (NV) and silicon vacancy (SiV) color centers in a commercially available, heteroepitaxial, wafer-sized, mm thick, single-crystal diamond. We observe single, native NV centers with a density of roughly 1 NV per μm3 and moderate coherence time (T2 = 5 μs) embedded in an ensemble of SiV centers. Using low temperature luminescence of SiV centers as a probe, we prove the high crystalline quality of the diamond especially close to the growth surface, consistent with a reduced dislocation density. Using ion implantation and plasma etching, we verify the possibility to fabricate nanostructures with shallow color centers rendering our material promising for fabrication of nanoscale sensing devices. As this diamond is available in wafer-sizes up to 100 mm, it offers the opportunity to up-scale diamond-based device fabrication.

Strongly anisotropic spin relaxation in the neutral silicon vacancy center in diamond

Color centers in diamond are a promising platform for quantum technologies, and understanding their interactions with the environment is crucial for these applications. We report a study of spin- lattice relaxation (T1) of the neutral charge state of the silicon vacancy center in diamond. Above 20 K, T1 decreases rapidly with a temperature dependence characteristic of an Orbach process, and is strongly anisotropic with respect to magnetic field orientation. As the angle of the magnetic field is rotated relative to the symmetry axis of the defect, T1 is reduced by over three orders of magnitude. The electron spin coherence time (T2) follows the same temperature dependence but is drastically shorter than T1. We propose that these observations result from phonon-mediated transitions to a low lying excited state that are spin conserving when the magnetic field is aligned with the defect axis, and we discuss likely candidates for this excited state.

Photoluminescence of silicon vacancy centres as conceptual indicator for the condition of diamond protection coatings

Due to the outstanding properties polycrystalline diamond coatings are used for wear protection on tools and work pieces. Thereby adhesive and abrasive wear as well as spalling of the coating can lead to damage and downtimes of the working machines. By depositing silicon doped multilayer diamond coatings, an indication of the condition of the coatings could be achieved. In this study the behaviour and transmission of the zero-phonon line of silicon vacancy centres is investigated in doped multilayer diamond coatings. The in-situ silicon doped diamond coatings were synthesized in use of an atmospheric laser-based plasma chemical vapour deposition. Photoluminescence measurements were performed with an excitation area of 18 mm2 and a wavelength of 248 nm. While the photoluminescence of the doped layers conceptually proves suitability as an indicator for the condition of the coating, the undoped diamond layers in the coatings show a high transmissivity to the zero-phonon line for the used parameters.

Effects of nitrogen on the interface density of states distribution in 4H-SiC metal oxide semiconductor field effect transistors: Super-hyperfine interactions and near interface silicon vacancy energy levels

The performance of silicon carbide (SiC)-based metal-oxide-semiconductor field-effect transistors (MOSFETs) is greatly enhanced by a post-oxidation anneal in NO. These anneals greatly improve effective channel mobilities and substantially decrease interface trap densities. In this work, we investigate the effect of NO anneals on the interface density of states through density functional theory (DFT) calculations and electrically detected magnetic resonance (EDMR) measurements. EDMR measurements on 4H-silicon carbide (4H-SiC) MOSFETs indicate that NO annealing substantially reduces the density of near interface SiC silicon vacancy centers: it results in a 30-fold reduction in the EDMR amplitude. The anneal also alters post-NO anneal resonance line shapes significantly. EDMR measurements exclusively sensitive to interface traps with near midgap energy levels have line shapes relatively unaffected by NO anneals, whereas the measurements sensitive to defects with energy levels more broadly distributed in the 4H-SiC bandgap are significantly altered by the anneals. Using DFT, we show that the observed change in EDMR linewidth and the correlation with energy levels can be explained by nitrogen atoms introduced by the NO annealing substituting into nearby carbon sites of silicon vacancy defects.

Luminescent diamond window of the sandwich type for X-ray visualization

A two-layered diamond plate is proposed as a transparent X-ray window visualizer. The plate consists of a thick substrate of a synthetic single-crystal high-pressure high-temperature (HPHT) diamond on which a thin $${\sim }10\, {\mu }m$$ optically active layer of chemical vapor deposition (CVD) diamond doped with silicon and nitrogen, and is epitaxially grown. The photoluminescent properties of the diamond sandwich plate were studied under the influence of X-ray radiation before and after treatment of the plate with high-energy electrons and its thermal annealing. It was established that broadband luminescence with a maximum near 500 nm, associated with defects of the HPHT diamond substrate, dominates before electron treatment. The electron irradiation and subsequent annealing of the plate completely suppressed the broadband luminescence and significantly (by more than two orders of magnitude) increased emission intensity of nitrogen-vacancy centers (NV) in the CVD diamond layer. As a result, the luminescence of neutrally charged NV centers with a zero-phonon line at 575 nm became dominant. No luminescence of the silicon-vacancy (SiV) centers in the CVD diamond film was detected. The first results demonstrating the two-layered diamond plate as an X-ray visualizer are presented.

Inducing interactions between quantum emitters

Quantum Optics The development of scalable quantum systems will require the ability to control the interactions between the individual quantum building blocks of the system. Evans et al. used a pair of silicon vacancy centers embedded in a diamond nanocavity to show that interactions between the quantum emitters can be mediated optically (see the Perspective by Lodahl). Such optical control provides a speed advantage as well as the potential to develop an integrated platform for future quantum communication and quantum networking. Science , this issue p. [662][1]; see also p. [646][2] [1]: /lookup/doi/10.1126/science.aau4691 [2]: /lookup/doi/10.1126/science.aav3076

Electronic structures and spectroscopic signatures of silicon-vacancy containing nanodiamonds

The presence of midgap states introduced by localized defects in wide-band-gap-doped semiconductors can strongly affect the electronic structure and optical properties of materials, generating a wide range of applications. Silicon-divacancy defects in diamond have been recently proposed for probing high-resolution pressure changes and performing quantum cryptography, making them good candidates to substitute for the more common nitrogen-vacancy centers. Using group-theory and ab initio electronic structure methods, the molecular origin of midgap states, zero-phonon line splitting, and size dependence of the electronic transitions involving the silicon-vacancy center is investigated in this paper. The effects of localized defects on the Raman vibrational and carbon $K$-edge x-ray absorption spectra are also explored for nanodiamonds. This paper presents an important analysis of the electronic and vibrational structures of nanosized semiconductors in the presence of midgap states due to localized defects, providing insight into possible mechanisms for modulating their optical properties.

Strongly inhomogeneous distribution of spectral properties of silicon-vacancy color centers in nanodiamonds

The silicon-vacancy (SiV) color center in diamond is a solid-state single photon emitter and spin quantum bit suited as a component in quantum devices. Here, we show that SiV centers in nanodiamonds exhibit a strongly inhomogeneous distribution with regard to the center wavelengths and linewidths of the zero-phonon-line (ZPL) emission at room temperature. We find that the SiV centers separate in two clusters: one group exhibits ZPLs with center wavelengths within a narrow range ≈730–742 nm and broad linewidths between 5 and 17 nm, whereas the second group comprises a very broad distribution of center wavelengths between 715 and 835 nm, but narrow linewidths from below 1 up to 4 nm. Supported by ab initio Kohn–Sham density functional theory calculations we show that the ZPL shifts of the first group are consistently explained by strain in the diamond lattice. Further, we suggest, that the second group showing the strongly inhomogeneous distribution of center wavelengths might be comprised of a new class of silicon-related defects. Whereas single photon emission is demonstrated for defect centers of both clusters, we show that emitters from different clusters show different spectroscopic features such as variations of the phonon sideband spectra and different blinking dynamics.

Phonon-Assisted Photoluminescence Up-Conversion of Silicon-Vacancy Centers in Diamond.

Phonon-assisted anti-Stokes photoluminescence (ASPL) up-conversion lies at the heart of optical refrigeration in solids. The thermal energy contained in the lattice vibrations is taken away by the emitted anti-Stokes photons' ASPL process, resulting in laser cooling of solids. To date, net laser cooling of solids is limited in rare-earth (RE)-doped crystals, glasses, and direct band gap semiconductors. Searching more solid materials with efficient phonon-assisted photoluminescence up-conversion is important to enrich optical refrigeration research. Here, we demonstrate the phonon-assisted PL up-conversion process from the silicon vacancy (SiV) center in diamond for the first time by studying ASPL spectra for the dependence of temperature, laser power, and excitation energy. Although net cooling has not been observed, our results show that net laser cooling might be eventually achieved in diamond by improving the external quantum efficiency to higher than 95%. Our work provides a promising route to investigate the laser cooling effect in diamond.

Accuracy of the Heyd-Scuseria-Ernzerhof hybrid functional to describe many-electron interactions and charge localization in semiconductors

Hybrid functionals, which mix a fraction of Hartree-Fock (HF) exchange with local or semilocal exchange, have become increasingly popular in quantum chemistry and computational materials science. Here, we assess the accuracy of the Heyd-Scuseria-Ernzerhof (HSE) hybrid functional to describe many-electron interactions and charge localization in semiconductors. We perform diffusion quantum Monte Carlo (DMC) calculations to obtain the accurate ground-state spin densities of the negatively charged (SiV)$^-$ and the neutral (SiV)$^0$ silicon-vacancy center in diamond, and of the cubic silicon carbide (3C-SiC) with an extra electron. We compare our DMC results with those obtained with the HSE functional and find a good agreement between both methods for (SiV)$^-$ and (SiV)$^0$, whereas the correct description of 3C-SiC with an extra electron crucially depends on the amount of HF exchange included in the functional. Also, we examine the case of the neutral Cd vacancy in CdTe, for which we assess the performance of HSE against the many-body \emph{GW} approximation for the description of the position of the defect states in the band gap.