Silicon Vacancy Research Articles

High-Yield Production of SiV-Doped Nanodiamonds for Spectroscopy and Sensing Applications.

Nanodiamonds (NDs) containing optically active centers have gained significant relevance as the material of choice for biological, optoelectronic, and quantum applications. However, current production methods lag behind their real needs. This study introduces two CVD-based approaches for fabricating NDs with optically active silicon-vacancy (SiV) color centers: bottom-up (BU) and top-down (TD) methods. The BU approach generates nanoporous diamond films with a core-shell structure, while the TD method employs molten-salt thermal etching to create uniform porous structures from nanocrystalline diamond films. Comprehensive characterization using advanced techniques revealed distinct morphologies and optical properties for each approach. The BU method yielded higher-quality diamond phases with top-surface incorporation of SiV centers, while the TD method demonstrated efficient nondiamond phase removal. Ultrasonic disintegration of both porous films produced NDs ranging from 40 to 500 nm, with unique morphologies characteristic of each approach. Photoluminescence measurements confirmed SiV centers (738 nm) in all NDs, exhibiting sensitivity to surface terminations, particularly in BU samples. Temperature-resolved spectroscopy shows the potential of the fabricated NDs for nano thermometry over a wide range of temperatures up to 100 °C. The zero-phonon line shows 0.022 ± 0.003 nm/K sensitivity, while the line width exhibits 0.068 ± 0.004 nm/K broadening. The presented BU and TD methods offer significant advantages over existing techniques, including streamlined production processes, high-yield ND synthesis with tailored properties, and the potential for scalable, cost-effective manufacturing.

Investigation of PCVSi− defect in 4H–SiC as a candidate for a qubit

Abstract Exploration of spin defects in semiconductors for possible qubits encourages the development of the quantum field. Silicon carbide (SiC) is a suitable platform to carry spin defects, due to its excellent electrical, mechanical and optical properties, together with its convenience for crystallographic growth and doping processes. In this study, a negatively charged phosphorus-vacancy (PCVSi −) defect, consisting of a silicon vacancy and nearby substitution of a phosphorus atom to a carbon atom in 4H–SiC, is investigated by first-principles calculations. This defect is demonstrated to possess a high spin (S = 1) with relatively low formation energy. Computed zero-phonon line energy and zero-field splitting parameters of this defect are close to those of neutral divacancy (VCVSi 0), negatively charged nitrogen-vacancy center (NCVSi −) and some other color centers, which indicate a similarity of both optical and spin properties among them. Moreover, the electron spin coherence time of this defect turns out to be 1.15–1.40 ms. Such a long coherence time provides the defect with reliability for quantum information processing. Our results show that the PCVSi − defect can be a promising candidate for a qubit.

Dynamics of charged and neutral silicon-vacancy color centers in electron-irradiated 28Si-doped single crystal chemical vapor deposition diamond upon annealing: Optical spectroscopy study

Diamond synthesis with silicon-vacancy (SiV) color centers is of high interest to nanophotonics and optical quantum technologies. The methods to control and/or maximize concentration of Si atoms incorporated in diamond lattice, and coupled to vacancies, together with improving crystallinity of diamond structure, are in demand. Here, we studied the effect of heat treatment of electron-irradiated single crystal CVD diamond doped with 28S isotope, on evolution of the neutral SiV0 and negatively charged SiV− centers. The crystal subjected to stepwise annealing at temperatures Tann from 200 °C to 1640 °C has been analyzed with photoluminescence (PL) and optical absorption spectroscopies at room and low-temperature (T = 5 K). We found a complex non-monotonous behavior of SiV0 and SiV− intensity both in absorption and PL, with sharp rise at Tann > 600 °C, reaching a maximum concentration peak, decline at 850 °C, and a repeated elevation to higher Tann, reflecting creation and annihilation processes of these defects. Moreover, we detected a group of seven lines of a Si-related defect in the range 828–871 nm, which strongly correlate with annealing dynamics of the SiV− and, especially, of SiV0 centers, and estimated the isotope spectral shift. In parallel, dynamics of other optical centers such as NV, R11 and GR1, in course of the annealing is traced. The controlled annealing opens the way to preparation of the SiV color centers with optimized optical properties, promising for quantum technologies.

Fabrication of silicon carbide color center nanoparticles by femtosecond laser ablation in liquid

Combined with the fabrication of low-dimensional materials, certain silicon carbide color centers can become excellent platforms for nano-optics, and be applied to quantum and biomedical fields. In this work, color center nanoparticles were prepared based on high purity semi-insulating silicon carbide substrate using liquid-assisted femtosecond laser machining. Effects of multi-pulse array ablation and line scanning fabrication were investigated, and parameters such as repetition frequency and pulse number were also optimized. We employed photoluminescence spectroscopy, field emission scanning electron microscopy and transient fluorescence spectroscopy to characterize optical properties and micromorphology of nanoparticles. The broadband photoluminescence within the range of 850–950 nm should be attributed to silicon vacancy color centers, and V1/V1’ zero-phonon lines were confirmed at low temperature. It is noted that the femtosecond laser annealing is critical for the luminescence enhancement of color center nanoparticles. The evolution of particles and cavitation bubbles during processing was elucidated. After optimization, silicon vacancy color center nanoparticles were prepared by multi-pulse (107) array ablation and 200 kHz pulse repetition frequency, with an average diameter of approximately 15 nm and an average density reaching 273.94 counts/μm2. The sample can be preserved stably in the form of nanoparticle solutions. Processing methods and corresponding conclusions of this study would be applicable to the femtosecond laser fabrication and micromorphology control of color center nanoparticles of various hard-brittle semiconductors.

Formation and properties of silicon vacancies in MPCVD-grown polycrystalline diamond

Formation and properties of silicon vacancies in MPCVD-grown polycrystalline diamond

Purcell Enhancement and Spin Spectroscopy of Silicon Vacancy Centers in Silicon Carbide Using an Ultrasmall Mode-Volume Plasmonic Cavity.

Silicon vacancy (VSi) centers in 4H-silicon carbide have emerged as a strong candidate for quantum networking applications due to their robust electronic and optical properties, including a long spin coherence lifetime and bright, stable emission. Here, we report the integration of VSi centers with a plasmonic nanocavity to Purcell enhance the emission, which is critical for scalable quantum networking. Employing a simple fabrication process, we demonstrate plasmonic cavities that support a nanoscale mode volume and exhibit an increase in the spontaneous emission rate with a measured Purcell factor of up to 48. In addition to investigating the optical resonance modes, we demonstrate an improvement in the optical stability of the spin-preserving resonant optical transitions relative to the radiation-limited value. The results highlight the potential of nanophotonic structures for advancing quantum networking technologies and emphasize the importance of optimizing emitter-cavity interactions for efficient quantum photonic applications.

Ultracoherent Gigahertz Diamond Spin-Mechanical Lamb Wave Resonators.

We report the development of an all-optical approach that excites the fundamental compression mode in a diamond Lamb wave resonator with an optical gradient force and detects the induced vibrations via strain coupling to a silicon vacancy center, specifically, via phonon sidebands in the optical excitation spectrum of the silicon vacancy. Sideband optical interferometry has also been used for the detection of in-plane mechanical vibrations, for which conventional optical interferometry is not effective. These experiments demonstrate a gigahertz fundamental compression mode with a Q factor of >107 at temperatures near 7 K, providing a promising platform for reaching the quantum regime of spin mechanics, especially phononic cavity quantum electrodynamics of electron spins.

Femtosecond laser controllable annealing for color centers based on ion-implanted silicon carbide substrate

As a representative of third-generation semiconductors, silicon carbide serves as a new platform for quantum nano-optics with readable paramagnetic color centers such as silicon vacancies. The potential applications include biomedical imaging, quantum sensing and micro/nano environment detection. Color centers are usually prepared based on ion-irradiated substrates, then annealed at high temperature to increase the yield. Currently, annealing furnaces have been the main method to heat the substrate and achieve annealing of the whole sample. However, further exploration is still necessary for fine processing requirements such as specialized annealing regions with certain shapes. In this work, we applied femtosecond laser to achieve controllable annealing at micron scale, based on silicon carbide substrate after ion injection. The whole process of point, line and pattern annealing was realized. The annealing area demonstrates enhanced photoluminescence, attributed to silicon vacancy color centers. Raman and photoluminescence spectra reveal that the annealing effect is primarily influenced by the number of pulses per unit area. The mechanism of femtosecond laser annealing was introduced. Finally, the controllable annealing areas with various shapes were prepared based on the comprehensive optimal parameters (100 kHz pulse repetition frequency, 105 point annealing pulses, 10 μm/s line scanning speed). This annealing strategy demonstrates excellent stability and uniformity, as well as micron scale accuracy. Additionally, the excited state lifetime of silicon vacancy was extracted and quantified. The result means that femtosecond laser annealing enhances the optical properties and quantum application potential of color centers. This work can be further extended to other semiconductors as well as patterned modification of local surface/planes at some depth, and helpful to explore the mechanism and applications of femtosecond laser annealing.

Evaluation of single silicon vacancy centers in nanodiamonds created by ion implantation at cryogenic temperatures

Abstract Silicon vacancy (SiV) centers in diamonds have attracted much attention because of their stability and narrow emission linewidth, and are promising for applications in quantum information technology. SiV-center-encapsulated nanodiamonds have also attracted much attention because of their potential to be coupled to various photonic devices. One efficient way to fabricate nanodiamonds that contain SiV centers is Si ion implantation into nanodiamonds. However, the evaluation of a single SiV center in a nanodiamond produced by this method at low temperatures has not been performed. In this study, we report on the optical properties of a single SiV center in a nanodiamond produced by ion implantation at cryogenic temperatures. The emission spectrum from a single SiV center ( g 2 ( 0 ) = 0.19 ) was observed with four distinct fine splittings of the zero-phonon line (ZPL) at 4 K. At an excitation power of 50 μ W, the full width at half maximum of the ZPL reached the spectrometer resolution limit (0.09 nm). The temperature dependence of the emission peak is consistent with that of the emission coming from an SiV center under high strain. The results obtained in this work suggest that nanodiamonds containing single SiV centers formed using this method will be an important building block for the realization of quantum information applications.

A DLTS analysis of alpha particle irradiated commercial 4H-SiC Schottky barrier diodes

4H-SiC Schottky barrier diodes (SBDs) were exposed to 5.4 MeV alpha particles with fluences of 2.55× 1011 cm−2, 5.11 × 1011 cm−2 and 7.67 × 1011 cm−2, respectively. Transmission electron microscopy (TEM) and energy dispersive spectroscopy (EDS) was used to determine the structure and cross-sectional elemental composition of the device, while current–voltage and capacitance–voltage profiling were used to determine the primary electrical device-characteristics before and after irradiation. EDS revealed the presence of a <1 μm Ti layer, covered by 5 μm Al layer, in intimate contact with the SiC. Deep level transient spectroscopy (DLTS), performed in the temperature range 15–310 K, revealed one dominant peak around 50 K (Ec - 0.07 eV) in the unirradiated samples. This peak showed asymmetry suggesting that it may consist of more than one defect. Notably, Z1/2, the carbon vacancy-related (Vc) defect commonly observed in as-grown n-type 4H-SiC, was not detected in the unirradiated reference sample. After irradiation, a broad peak emerged around 280 K (at 80 Hz), most likely Z1/2, having a shoulder around 180 K, was detected. Increasing the fluence resulted in a corresponding decrease in the concentration of the electron trap observed around 50 K (Ec - 0.07 eV), while the concentration increases for the defect detected around 280 K. Notably, the concentration of Z1/2 was found to be strongly fluence dependent and linked to what we believe is a related to a silicon vacancy transition, labelled S1/2 in literature. Laplace DLTS confirmed that the peak observed around 50 K is composed of multiple defects.

Improving the creation of SiV centers in diamond via sub-μs pulsed annealing treatment

Silicon-vacancy (SiV) centers in diamond are emerging as promising quantum emitters in applications such as quantum communication and quantum information processing. Here, we demonstrate a sub-μs pulsed annealing treatment that dramatically increases the photoluminescence of SiV centers in diamond. Using a silane-functionalized adamantane precursor and a laser-heated diamond anvil cell, the temperature and energy conditions required to form SiV centers in diamond were mapped out via an optical thermometry system with an accuracy of ±50 K and a 1 μs temporal resolution. Annealing scheme studies reveal that pulsed annealing can obviously minimize the migration of SiV centers out of the diamond lattice, and a 2.5-fold increase in the number of emitting centers was achieved using a series of 200-ns pulses at a 50 kHz repetition rate via acousto-optic modulation. Our study provides a novel pulsed annealing treatment approach to improve the efficiency of the creation of SiV centers in diamond.

Optical Ionization of Qubits and their Silent Charge States

Color centers in the technologically mature material silicon carbide are candidates for the implementation of quantum applications. Chargestate control and electrical read-out of qubits includes spin-to-charge conversion via optical excitation and subsequent ionization. In this work we address the dominant photoionization mechanism and the photophysical properties of the ionized silicon vacancy in 4H SiC using ab initio theory. We find that its nominally dark chargestates are infrared emitters.

Spin-Orbit Coupling of Color Centers for Quantum Applications

Color centers in 4H-SiC and diamond are candidates for single photon sources and qubits for the implementation of quantum applications. The CI-cRPA method is able to correctly reproduce the structure of the underlying highly correlated wave functions for low and high spin multiplets. Aiming for a more complete understanding of spin-orbit mediated intersystem crossing between such states, we have extended CI-cRPA by a first order treatment of the spin-orbit interactions. We present preliminary results for intercrossing matrix elements and contributions of spin-orbit coupling to the zero field splitting of the silicon vacancy and di-vacancy in 4H-SiC, as well as the NV center in diamond using this approach.

The silicon vacancy centers in SiC: determination of intrinsic spin dynamics for integrated quantum photonics

The negatively charged silicon vacancy center (VSi−\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\\rm{V}}}_{{\\rm{Si}}}^{-}$$\\end{document}) in silicon carbide (SiC) is an emerging color center for quantum technology covering quantum sensing, communication, and computing. Yet, limited information currently available on the internal spin-optical dynamics of these color centers prevents us from achieving the optimal operation conditions and reaching the maximum performance especially when integrated within quantum photonics. Here, we establish all the relevant intrinsic spin dynamics of the VSi−\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{\\rm{V}}}_{{\\rm{Si}}}^{-}$$\\end{document} center at cubic lattice site (V2) in 4H-SiC by an in-depth electronic fine structure modeling including the intersystem-crossing and deshelving mechanisms. With carefully designed spin-dependent measurements, we obtain all the previously unknown spin-selective radiative and non-radiative decay rates. To showcase the relevance of our work for integrated quantum photonics, we use the obtained rates to propose a realistic implementation of time-bin entangled multi-photon GHZ and cluster state generation. We find that up to three-photon GHZ or cluster states are readily within reach using the existing nanophotonic cavity technology.

Generation of macroscopic entanglement in ensemble systems based on silicon vacancy centers

Abstract Entanglement in macroscopic systems, as a fundamental quantum resource, has been utilized to propel the advancement of quantum technology and probe the boundary between the quantum and classical realms. This study focuses on a unique hybrid quantum system comprising of an ensemble of silicon vacancy (SiV) centers coupled to phononic waveguides in diamond via strain interactions. By employing two sets of time-dependent, non-overlapping driving fields, we investigate the generation process and dynamic properties of macroscopic quantum entanglement, providing fresh insights into the behavior of such hybrid quantum systems. Furthermore, it paves the way for new possibilities in utilizing quantum entanglement as an information carrier in quantum information processing and quantum communication.

Overcoming Temperature Limits in the Optical Cooling of Solids Using Light-Dressed States.

Laser cooling of solids currently has a temperature floor of 50-100K. We propose a method that could overcome this using defects, such as diamond color centers, with narrow electronic manifolds and bright optical transitions. It exploits the dressed states formed in strong fields which extend the set of phonon transitions and have tunable energies. This allows an enhancement of the cooling power and diminishes the effect of inhomogeneous broadening. We demonstrate these effects theoretically for the silicon vacancy and the germanium vacancy, and discuss the role of background absorption, phonon-assisted emission, and nonradiative decay.

Formation and stability of point defect color centers in 6H silicon carbide

Point defect color centers acting as single-photon emitters are promising for quantum technology applications and have been extensively studied, e.g., in the 4H polytype of silicon carbide (SiC). However, the physics of such color centers in other SiC polytypes is much less explored. Herein, we study the formation and thermal stability of such color centers in 6H-SiC using photoluminescence spectroscopy. The emissions from typical single-photon emitters, such as silicon vacancies, divacancies, and carbon antisite-vacancy pairs in 6H-SiC, were monitored as a function of the proton irradiation fluence and post-irradiation annealing, and compared to that in 4H-SiC. Overall, at the background of similarities between the emission behavior in 4H- and 6H-SiC polytypes, we observed prominent differences; e.g., for the thermal stability of the carbon antisite-vacancy pair, which exhibited maximized emissions upon 300 and 900 °C anneals in 4H- and 6H-SiC, respectively. Moreover, we observed a range of defect emission signatures not previously reported for 6H-SiC in the literature and discussed their potential origin in the context of the thermal stability. For example, among the PL-lines in 6H-SiC, we detected periodically repeatable emission signatures, resembling the so-called L-lines recently reported in 4H-SiC, even though their exact origin has not yet been settled in the literature. Thus, we use color centers comparison in different polytypes to better understand the nature of the single-photon emitters in SiC.

Selection rules in the excitation of the divacancy and the nitrogen-vacancy pair in 4 H - and 6 H -SiC

In this study, we address selection rules with respect to the polarization of the optical excitation of two color centers in 4H−SiC and 6H−SiC with potential for applications in quantum technology, the divacancy and the nitrogen-vacancy pair. We show that the photoluminescence of the axial configurations of higher symmetry (C3v) than the basal ones (C1h) can be canceled using any excitation (resonant or nonresonant) with polarization parallel to the crystal axis (EL||c). The polarization selection rules are determined using group-theoretical analysis and simple physical arguments showing that phonon-assisted absorption with EL||c is prohibited despite being formally allowed by group theory. A comparison with the selection rules for the silicon vacancy, another defect with C3v symmetry, is also carried out. Using the selection rules, we demonstrate selective excitation of only one basal divacancy configuration in 4H−SiC, the PL3 line, and discuss the higher contrast and increased Debye-Waller factor in the selectively excited spectrum. Published by the American Physical Society 2024

High Q-Factor Diamond Optomechanical Resonators with Silicon Vacancy Centers at Millikelvin Temperatures.

Phonons are envisioned as coherent intermediaries between different types of quantum systems. Engineered nanoscale devices, such as optomechanical crystals (OMCs), provide a platform to utilize phonons as quantum information carriers. Here we demonstrate OMCs in diamond designed for strong for interactions between phonons and a silicon vacancy (SiV) spin. Using optical measurements at millikelvin temperatures, we measure a line width of 13 kHz (Q-factor of ∼4.4 × 105) for a 6 GHz acoustic mode, a record for diamond in the GHz frequency range and within an order of magnitude of state-of-the-art line widths for OMCs in silicon. We investigate SiV optical and spin properties in these devices and outline a path toward a coherent spin-phonon interface.

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.