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arXiv:2509.06500 · Physical review. B./Physical review. B

Tuning of SiV quantum emission in nitrogen-doped nanodiamonds by dual-color excitation

Alexander A. Zhivopistsev, Alexey M. Romshin, Alexander V. Gritsienko, Dmitrii G. Pasternak, R. Kh. Bagramov, Vladimir P. Filonenko, Fedor M. Maksimov, A. I. Chernov, A. M. Skomorokhov, Alexander A. Rodionov, Н. И. Каргин, Igor I. Vlasov

Published Dec 31, 2025• 1 citation
arXivHTMLPDF

Abstract

The charge dynamics of silicon-vacancy (SiV) centers have been investigated for the first time in high-pressure high-temperature nanodiamonds (NDs) with varying concentrations of substitutional nitrogen (Ns). We demonstrate a controlled sixfold enhancement of SiV- photoluminescence (PL) under dual-color excitation, consisting of strong red (~660 nm) illumination combined with weak green (~530 nm) excitation. The measured dependencies of SiV- PL lifetime and intensity on excitation wavelength, together with the enhancement dependence on Ns concentration in the studied nanodiamonds, provide unambiguous evidence of the involvement of donor nitrogen in SiV-emission dynamics. Saturation curves and second-order PL intensity correlation measurements further indicate suppression of the population of the optically inactive SiV2- state upon the addition of green excitation. These results unlock a practical pathway toward engineering optically-controlled and scalable quantum emitters based on SiV-luminescent diamond nanoparticles.

DOI
10.1103/bckz-c6bc

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The charge dynamics of silicon-vacancy (SiV) centers have been investigated for the first time in high-pressure high-temperature nanodiamonds (NDs) with varying concentrations of substitutional nitrogen (Ns). We demonstrate a controlled sixfold enhancement of SiV- photoluminescence (PL) under dual-color excitation, consisting of strong red (~660 nm) illumination combined with weak green (~530 nm) excitation. The measured dependencies of SiV- PL lifetime and intensity on excitation wavelength, together with the enhancement dependence on Ns concentration in the studied nanodiamonds, provide unambiguous evidence of the involvement of donor nitrogen in SiV-emission dynamics. Saturation curves and second-order PL intensity correlation measurements further indicate suppression of the population of the optically inactive SiV2- state upon the addition of green excitation. These results unlock a practical pathway toward engineering optically-controlled and scalable quantum emitters based on SiV-luminescent diamond nanoparticles.
Group IV vacancy color centers in diamond are promising spin-photon interfaces with strong potential for applications in photonic quantum technologies. Reliable methods for controlling and stabilizing their charge state are urgently needed for scaling to multiqubit devices. Here, we manipulate the charge state of silicon vacancy (SiV) ensembles by combining luminescence and photocurrent spectroscopy. We controllably convert the charge state between the optically active SiV − and dark SiV 2− with megahertz rates and >90% contrast by judiciously choosing the local potential applied to in-plane surface electrodes and the laser excitation wavelength. We observe intense SiV − photoluminescence under hole capture, measure the intrinsic conversion time from the dark SiV 2− to the bright SiV − to be 36.4(67) ms, and demonstrate how it can be enhanced by a factor of 10 5 via optical pumping. Moreover, we obtain previously unknown information on the defects that contribute to photoconductivity, indicating the presence of substitutional nitrogen and divacancies.
Synthetic high-pressure high-temperature (HPHT) microdiamonds demonstrate strong resonant-like enhancement of the NV− photoluminescence (PL) at unexpectedly low concentration of the substitutional nitrogen atoms (NS) of 90 ppm, which is significantly smaller than the ∼250 ppm characteristic for conventional HPHT synthesis. The EPR, Raman, and luminescent spectroscopies, including time-resolved PL, provide evidence that this is due to competition between the increase in PL with increasing concentration of the NV− centers and nonradiative deactivation of these centers by defects induced by the NS in the diamond crystal lattice. It is suggested that the intensity of the NV− center emission can be optimized by the appropriate choice of nitrogen doping concentration which does not substantially disrupt the diamond crystal lattice.
We use a simple and effective experimental method for determining the radiative quantum yield of single silicon-vacancy centers (SiV) in nanometric-sized diamonds (NDs). It is based on variations in the luminescence lifetimes of SiVs induced by a controlled change in the NDs' dielectric environment. The deposition of a high refractive index immersion oil on a thin polymer sample containing NDs with an average size of 20 nm induces a noticeable shortening of SiV lifetimes, a clear signature of a strong radiative contribution to the decays. While SiV centers were generally considered to be weak quantum emitters, we demonstrate that single SiV centers in nanodiamonds have a quantum efficiency up to 60%, under ambient conditions. This quantum efficiency is very similar to that of the negatively charged nitrogen-vacancy centers, which we measured using the same approach. This feature makes single SiV attractive as bright, high-purity single-photon sources for quantum technologies.
Abstract Nitrogen-vacancy (NV) and silicon-vacancy (SiV) color defects in diamond are promising systems for applications in quantum technology. The NV and SiV centers have multiple charge states, and their charge states have different electronic, optical and spin properties. For the NV centers, most investigations for quantum sensing applications are targeted on the negatively charged NV (NV−), and it is important for the NV centers to be in the NV− state. However, it is known that the NV centers are converted to the neutrally charged state (NV0) under laser excitation. An energetically favorable charge state for the NV and SiV centers depends on their local environments. It is essential to understand and control the charge state dynamics for their quantum applications. In this work, we discuss the charge state dynamics of NV and SiV centers under high-voltage nanosecond pulse discharges. The NV and SiV centers coexist in the diamond crystal. The high-voltage pulses enable manipulating the charge states efficiently. These voltage-induced changes in charge states are probed by their photoluminescence spectral analysis. The analysis result from the present experiment shows that the high-voltage nanosecond pulses cause shifts of the chemical potential and can convert the charge states of NV and SiV centers with the transition rates of ∼MHz. This result also indicates that the major population of the SiV centers in the sample is the doubly negatively charged state (SiV2−), which is often overlooked because of its non-fluorescent and non-magnetic nature. This demonstration paves a path for a method of rapid manipulation of the NV and SiV charge states in the future.
Silicon-vacancy (SiV) centers in diamond are gaining an increased interest for application, such as in quantum technologies and sensing. Due to the strong luminescence concentrated in its sharp zero-phonon line at room temperature, SiV centers are being investigated as single-photon sources for quantum communication, and also as temperature probes for sensing. Here, we discussed strategies for the fabrication of SiV centers in diamond based on Si-ion implantation followed by thermal activation. SiV color centers in high-quality single crystals have the best optical properties, but polycrystalline micro and nanostructures are interesting for applications in nano-optics. Moreover, we discuss the photoluminescence properties of SiV centers in phosphorous-doped diamond, which are relevant for the creation of electroluminescent devices, and nanophotonics strategies to improve the emission characteristics of the SiV centers. Finally, the optical properties of such centers at room and high temperatures show the robustness of the center and give perspectives for temperature-sensing applications.
Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV-) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV- to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV- charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower Ns0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T1 spin relaxation times of 3.2 ±\pm± 0.7 ms and 4.7 ±\pm± 1.6 ms, respectively, compared to 0.17 ±\pm± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T1 spin relaxation properties.