Silicon-vacancy Centers Research Articles

Diamond composite with embedded YAG:Ce nanoparticles as a source of fast X-ray luminescence in the visible and near-IR range

The diamond composite materials with embedded yttrium-aluminum garnet doped with cerium (YAG:Ce) nanoparticles have been produced by microwave plasma-assisted chemical vapor deposition (CVD). Nanoparticles were synthesized by co-precipitation from an aqueous solution while CVD diamond served as the transparent matrix with high thermal conductivity, hardness, and resistivity to radiation damage. The composite films show high-intensity X-ray luminescence (XRL) with a broad band peaking around the wavelength of 550 nm (5d → 4f transition in Ce3+ ion), and a narrow peak of silicon-vacancy (Si–V) centers at 738 nm. The characteristic decay time was measured at τCe < 50 ns for cerium emission and at τSiV∼1 ns for Si–V centers. Excitation spectra of both luminescence types measured near yttrium K-edge (17.1 keV) show a strong correlation, attributed to the excitation of Si–V luminescence by photoelectrons ejected from YAG:Ce nanoparticles. The discovered phenomenon suggests a new way to control X-ray visualization by luminescent diamond composites for fast X-ray detectors and screens.

Coupling spins to nanomechanical resonators: Toward quantum spin-mechanics

Spin-mechanics studies interactions between spin systems and mechanical vibrations in a nanomechanical resonator and explores their potential applications in quantum information processing. In this review, we summarize various types of spin-mechanical resonators and discuss both the cavity-QED-like and the trapped-ion-like spin-mechanical coupling processes. The implementation of these processes using negatively charged nitrogen vacancy and silicon vacancy centers in diamond is reviewed. Prospects for reaching the full quantum regime of spin-mechanics, in which quantum control can occur at the level of both a single spin and a single phonon, are discussed with an emphasis on the crucial role of strain coupling to the orbital degrees of freedom of the defect centers.

Confocal photoluminescence characterization of silicon-vacancy color centers in 4H-SiC fabricated by a femtosecond laser

Silicon-vacancy (VSi) centers in silicon carbide (SiC) are expected to serve as solid qubits, which can be used in quantum computing and sensing. As a new controllable color center fabrication method, femtosecond (fs) laser writing has been gradually applied in the preparation of VSi in SiC. In this study, 4H-SiC was directly written by an fs laser and characterized at 293 K by atomic force microscopy, confocal photoluminescence (PL), and Raman spectroscopy. PL signals of VSi were found and analyzed using 785 nm laser excitation by means of depth profiling and two-dimensional mapping. The influence of machining parameters on the VSi formation was analyzed, and the three-dimensional distribution of VSi defects in the fs laser writing of 4H-SiC was established.

Optically Detected Magnetic Resonance in Neutral Silicon Vacancy Centers in Diamond via Bound Exciton States.

Neutral silicon vacancy (SiV^{0}) centers in diamond are promising candidates for quantum networks because of their excellent optical properties and long spin coherence times. However, spin-dependent fluorescence in such defects has been elusive due to poor understanding of the excited state fine structure and limited off-resonant spin polarization. Here we report the realization of optically detected magnetic resonance and coherent control of SiV^{0} centers at cryogenic temperatures, enabled by efficient optical spin polarization via previously unreported higher-lying excited states. We assign these states as bound exciton states using group theory and density functional theory. These bound exciton states enable new control schemes for SiV^{0} as well as other emerging defect systems.

Group-III quantum defects in diamond are stable spin-1 color centers

Color centers in diamond have emerged as leading solid-state artificial atoms for a range of quantum technologies, from quantum sensing to quantum networks. Concerted research activities are now underway to identify new color centers that combine stable spin and optical properties of the nitrogen vacancy (NV$^-$) with the spectral stability of the silicon vacancy (SiV$^-$) centers in diamond, with recent research identifying other group IV color centers with superior properties. In this Letter, we investigate a new class of diamond quantum emitters from first principles, the group III color centers, which we show to be thermodynamically stable in a spin-1, electric-field insensitive structure. From ab initio electronic structure methods, we characterize the product Jahn-Teller (pJT) effect present in the excited state manifold of these group III color centers, where we capture symmetry-breaking distortions associated with strong electron-phonon coupling. These predictions can guide experimental identification of group III vacancy centers and their use in applications in quantum information science and technology.

Robust Detection of High-Frequency Signals at the Nanoscale

We present a method relying on shortcuts to adiabaticity to achieve quantum detection of high frequency signals at the nanoscale in a robust manner. More specifically, our protocol delivers tailored amplitudes and frequencies for control fields that, firstly, enable the coupling of the sensor with high-frequency signals and, secondly, minimise errors that would otherwise spoil the detection process. To exemplify the method, we particularise to detection of signals emitted by fast-rotating nuclear spins with nitrogen vacancy center quantum sensors. However, our protocol is straightforwardly applicable to other quantum devices such as silicon vacancy centers, germanium vacancy centers, or divacancies in silicon carbide.

Photoluminescence study on the optical properties of silicon-vacancy centre in diamond

The optical properties of a silicon-vacancy (Si–V) centre were studied using photoluminescence (PL), including the temperature (80 K–270 K) and excitation power (2.25 W-22.5 mW)-dependent PL measurements and the effect of electron irradiation on the PL signal. The intensity decrease, red shift, and broadening of the line width with increasing temperature were fitted nonlinearly. The thermal quenching activation energy (49.59 meV), Huang-Rhys factor (0.049), and average phonon energy (42.09 meV) of the Si–V centre were obtained using suitable physical formulas. For the excitation power dependence, only the PL intensity of Si–V centre was sub-linear with the increasing power, the radiative recombination was dominated and the impact of Auger recombination was negligible. In addition, Fermi level shifted below the ground state level of Si–V in irradiation region due to the introduction of neutral single vacancy (GR1) centre, the PL signal of the Si–V centre was suppressed.

Bright silicon vacancy centers in diamond/SiC composite films synthesized by a MPCVD method

SiC is always produced forming diamond/SiC composite films owing to the oversaturated doping of Si atoms during the preparation of high emission SiV centers. As a higher refractive index material (n = 2.72), the presence of SiC could possibly lead to inefficient photo-luminescent (PL) collection of SiV centers with total internal reflection. In order to understand such effect, different diamond/SiC films were deposited in a 915 MHz microwave plasma CVD (MPCVD) using the reactive gas of tetramethylsilane (TMS). The microstructure and photoluminescence of SiV centers were systematically investigated. It is found that the addition of TMS gas leads to the formation of cubic β-SiC and the refinement of diamond crystals. At the TMS gas flow of 5 sccm, the concentration of β-SiC is about 10% and the average diamond size is about 98 nm. The film exhibits the optimized PL emission of SiV centers, with the ratio of SiV PL to diamond Raman peak being 21.4. Increasing TMS gas flow leads to the increase of the concentration of β-SiC and the deterioration of PL emission of SiV centers. These results reveal that the introduction of TMS gas at a low flow advances the formation of diamond/SiC film containing high-brightness SiV centers.

Electronic structure and magneto-optical properties of silicon-nitrogen-vacancy complexes in diamond

The silicon-vacancy (SiV) and nitrogen-vacancy (NV) centers in diamond are commonly regarded as prototypical defects for solid-state quantum information processing. Here we show that when silicon and nitrogen are simultaneously introduced into the diamond lattice these defects can strongly interact and form larger complexes. Nitrogen atoms strongly bind to Si and SiV centers and complex formation can occur. Using a combination of hybrid density functional theory (DFT) and group theory, we analyze the electronic structure and provide various useful physical properties, such as hyperfine structure, quasi-local vibrational modes, and zero-phonon line, to enable experimental identification of these complexes. We demonstrate that the presence of substitutional silicon adjacent to nitrogen significantly shifts the donor level toward the conduction band, resulting in an activation energy for the SiN center that is comparable to phosphorus. We also find that the neutral SiNV center is of particular interest due to its photon emission at $\sim$1530 nm, which falls within the C band of telecom wavelengths, and its paramagnetic nature. In addition, the optical transition associated with the SiNV$^0$ color center exhibits very small electron--phonon coupling (Huang--Rhys factor~=~0.78) resulting in high quantum efficiency (Debye-Waller factor = 46\%) for single-photon emission. These features render this new center very attractive for potential application in scalable quantum telecommunication networks.

Coupling silicon vacancy centers in a thin diamond membrane to a silica optical microresonator.

We report the development of a composite cavity QED system, in which silicon vacancy centers in a diamond membrane as thin as 100 nm couple to optical whispering gallery modes (WGMs) of a silica microsphere with a diameter of order 50 µm. The membrane induces a linewidth broadening of 3 MHz for equatorial and off-resonant WGMs, while the overall linewidth of the composite system remains below 40 MHz. Photoluminescence experiments in the cavity QED setting demonstrate the efficient coupling of optical emissions from silicon vacancy centers into the WGMs. Additional analysis indicates that the composite system can be used to achieve the good cavity limit in cavity QED, enabling an experimental platform for applications such as state transfer between spins and photons.

Optical manipulation of the negative silicon-vacancy center in diamond

The silicon-vacancy center in diamond has recently attracted significant attention as a candidate for quantum information processing as it overcomes many of the optical issues present in the nitrogen-vacancy center. Historically it has been hampered by short dephasing times; however the recent development of high-purity samples at low temperatures resolves this issue. Hence it is timely to explore whether silicon-vacancy centers are useful for quantum tasks beyond single-photon sources. Here we investigate the potential of the silicon-vacancy center to realize two important operations required for quantum information processing: high-efficiency projective measurement and efficient single-qubit rotations. Due to its similar nature, the germanium-vacancy center is discussed as a point of comparison.

Dissipative generation of steady-state entanglement of two separated SiV$$^{-}$$ centers coupled to photonic crystal cavities

We propose an efficient scheme for the dissipative generation of steady-state entanglement of two negatively charged silicon-vacancy (SiV $$^{-}$$ ) centers, which are coupled to two separated photonic crystal cavities, respectively. With the external driving fields to tailor the desired interaction between the Zeeman-split lower orbital branches of the ground states of the SiV $$^{-}$$ centers and the cavity fields, we show that the heavily damped cavities can induce an effective quantum reservoir coupled to the two SiV $$^{-}$$ centers. Based on a form of quantum reservoir engineering, the two SiV $$^{-}$$ centers can be cooled down to an entangled state at stationary state. Our scheme has the distinct feature that the decay of the cavities as resource is utilized for producing the steady-state entanglement, which does not need to exactly prepare the initial state of the system. The present work may open up promising perspectives for realizing quantum networks and quantum information processing with solid-state SiV $$^{-}$$ centers in nanophotonic structures.

Cryogenic platform for coupling color centers in diamond membranes to a fiber-based microcavity

We operate a fiber-based cavity with an inserted diamond membrane containing ensembles of silicon vacancy centers (SiV{}^{-}) at cryogenic temperatures ge 4~K. The setup, sample fabrication and spectroscopic characterization are described, together with a demonstration of the cavity influence by the Purcell effect. This paves the way towards solid-state qubits coupled to optical interfaces as long-lived quantum memories.

Fourier Transform Limited Linewidth of Optical Transitions in Single SiV Centers in “Adamantane” Nanodiamonds

Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~103) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.

Photoluminescence studies of nitrogen-vacancy and silicon-vacancy centers transformation in CVD diamond

In this study, the low-temperature micro-photoluminescence (PL) technology was employed to investigate the transformation of nitrogen-vacancy (NV), silicon-vacancy (SiV) centers in diamond crystal. Results showed that the NV and SiV luminescence were controlled by electron irradiation followed by thermal annealing. Both centers vanished together with the emergence of neutral single vacancy (GR1 center) after 200 keV electron irradiation. Interstitial related defects and vacancies were activated to diffuse by annealing (above ∼400 and 700 °C, respectively). The vacancies migrated to be captured by N and Si atoms due to the strain fields around the atoms attracted vacancies, and the NV and SiV centers appeared again in the PL spectra. In addition, compared the annealing behavior with NV center, the new emission at 639.7 nm was attributed to the nitrogen combined with carbon interstitials.

Doubly charged silicon vacancy center, Si-N complexes, and photochromism in N and Si codoped diamond

We report the first experimental observation of a doubly-charged defect in diamond, SiV2-, in silicon and nitrogen co-doped samples. We measure spectroscopic signatures we attribute to substitutional silicon in diamond, and identify a silicon-vacancy complex decorated with a nearest-neighbor nitrogen, SiVN, supported by theoretical calculations. Samples containing silicon and nitrogen are shown to be heavily photochromic, with the dominant visible changes due to the loss of SiV0/- and gain in the optically-inactive SiV2-.

Spin-controlled generation of indistinguishable and distinguishable photons from silicon vacancy centres in silicon carbide

Quantum systems combining indistinguishable photon generation and spin-based quantum information processing are essential for remote quantum applications and networking. However, identification of suitable systems in scalable platforms remains a challenge. Here, we investigate the silicon vacancy centre in silicon carbide and demonstrate controlled emission of indistinguishable and distinguishable photons via coherent spin manipulation. Using strong off-resonant excitation and collecting zero-phonon line photons, we show a two-photon interference contrast close to 90% in Hong-Ou-Mandel type experiments. Further, we exploit the system’s intimate spin-photon relation to spin-control the colour and indistinguishability of consecutively emitted photons. Our results provide a deep insight into the system’s spin-phonon-photon physics and underline the potential of the industrially compatible silicon carbide platform for measurement-based entanglement distribution and photonic cluster state generation. Additional coupling to quantum registers based on individual nuclear spins would further allow for high-level network-relevant quantum information processing, such as error correction and entanglement purification.

Spectroscopic signatures of electron-phonon coupling in silicon-vacancy centers in diamond

Vacancy centers in diamond have proven to be a viable solid-state platform for quantum coherent opto-electronic applications. Among the variety of vacancy centers, silicon-vacancy (SiV) centers have recently attracted much attention as an inversion-symmetric system that is less susceptible to electron-phonon interactions. Nevertheless, phonon-mediated processes still degrade the coherent properties of SiV centers, however characterizing their electron-phonon coupling is extremely challenging due to their weak spectroscopic signatures and remains an open experimental problem. In this paper we theoretically investigate signatures of electron-phonon coupling in simulated linear and nonlinear spectra of SiV centers. We demonstrate how even extremely weak electron-phonon interactions, such as in SiV centers, may be completely characterized via nonlinear spectroscopic techniques and even resolved between different fine-structure transitions.

Effects of air annealing on microstructure and optical properties of HFCVD grown microcrystalline diamond thin films

In this report, we investigate the annealing effects on microcrystalline diamond thin films of 1 μm thickness grown on silicon substrate by hot filament chemical vapor deposition technique. Annealing is important from the perspective of etching away the non-diamond/graphitic phase situated mainly at the grain boundaries to yield a high-quality continuous diamond film with higher sp3 %. From the Raman spectroscopy and also from the morphology of the films, we could see that with annealing in air, the degradation of the sp2 component sets in at around 500 °C leaving behind the sp3 component in the films, however the films are completely oxidised with annealing at 700 °C. Our results show that annealing at 500 °C has been able to etch away the sp2 phase efficiently as evident from the Raman spectroscopic analysis making the characteristic diamond peak more intense compared to graphitic peaks and also led to the decrease in FWHM of the diamond peak. The photoluminescence properties reveal the presence of silicon-vacancy centers in the film whose zero-phonon line (ZPL) shows a drastic decrease in the FWHM as we anneal at higher temperatures of more than 700 °C.

Observation of a 1.979-eV spectral line of a germanium-related color center in microdiamonds and nanodiamonds

Color centers in diamond are considered as a platform for quantum computing and communications, biomedical markers, and nanosensors. Negatively charged split-vacancy centers have outstanding properties due to bright and almost monochromatic luminescence, but they have poor spin coherence and relaxation times. This drawback is believed to be absent in the neutral charge state of the defects. So far only the neutral silicon-vacancy center has been observed in luminescence and absorption spectra. Here we report the observation of its germanium-based analog in luminescence spectra with the zero-phonon line (ZPL) at 1.979 eV in samples containing negatively charged ${\mathrm{GeV}}^{\ensuremath{-}}$ centers. The relationship between the center and Ge dopant is unambiguously confirmed by studies of $^{12}\mathrm{C}$ diamonds containing $^{70}\mathrm{Ge}$, $^{73}\mathrm{Ge}$, or $^{76}\mathrm{Ge}$ isotopes. The intensity ratio of the ZPL of these centers varies with the crystal size, and the intensity of the ${\mathrm{GeV}}^{0}$ centers reaches its maximum in samples 150 nm in size. In the vibronic sideband of this center the local vibrational mode with an energy of 23 meV was identified. The density functional theory calculations yield a ZPL energy value of the ${\mathrm{GeV}}^{0}$ center which is 150 meV higher than the experimentally observed one and matches the values of its relaxational energy as well as the local phonon mode frequency.