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arXiv:1812.06534 · ACS Applied Nano Materials

Single Silicon Vacancy Centers in 10 nm Diamonds for Quantum Information Applications

Stepan V. Bolshedvorskii, Anton I. Zeleneev, Vadim V. Vorobyov, Vladimir V. Soshenko, Olga R. Rubinas, Leonid A. Zhulikov, Pavel A. Pivovarov, Vadim N. Sorokin, Andrey N. Smolyaninov, Liudmila F. Kulikova, Anastasiia S. Garanina, Sergey G. Lyapin, V. Agafonov, Rustem E. Uzbekov, Валерий Александрович Давыдов, Alexey V. Akimov

Published Jul 8, 2019• 36 citations
arXivHTMLPDF

Abstract

Ultrasmall (about 10 nm), low-strain, artificially produced diamonds with an internal, active color center have substantial potential for quantum information processing and biomedical applications. Thus, it is of great importance to be able to artificially produce such diamonds. Here, we report on the high-pressure, high-temperature synthesis of such nanodiamonds about 10 nm in size and containing an optically active, single silicon-vacancy color center. Using special sample preparation technique, we were able to prepare samples containing single nanodiamonds on the surface. By correlating atomic-force microscope images and confocal optical images, we verified the presence of optically active color centers in single nanocrystals, and using second-order correlation measurements, we proved the single-photon emission statistics of these nanodiamonds. These color centers have nonblinking, spectrally narrow emission with narrow distribution of spectral width and positions of zero-phonon line, thus proving the high quality of the nanodiamonds produced.

DOI
10.1021/acsanm.9b00580

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Ultrasmall (about 10 nm), low-strain, artificially produced diamonds with an internal, active color center have substantial potential for quantum information processing and biomedical applications. Thus, it is of great importance to be able to artificially produce such diamonds. Here, we report on the high-pressure, high-temperature synthesis of such nanodiamonds about 10 nm in size and containing an optically active, single silicon-vacancy color center. Using special sample preparation technique, we were able to prepare samples containing single nanodiamonds on the surface. By correlating atomic-force microscope images and confocal optical images, we verified the presence of optically active color centers in single nanocrystals, and using second-order correlation measurements, we proved the single-photon emission statistics of these nanodiamonds. These color centers have nonblinking, spectrally narrow emission with narrow distribution of spectral width and positions of zero-phonon line, thus proving the high quality of the nanodiamonds produced.
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.
Nanodiamonds containing single tin-vacancy (SnV) centers have the potential for integration into nanophotonic devices employed in quantum technologies such as quantum sensing, quantum information processing and quantum communication. The present study assessed single SnV centers in nanodiamonds less than 10 nm in size. Such centers were generated by implanting Sn ions into size-selected small nanodiamonds followed by high-temperature annealing. A sharp emission peak with a line width of 2.6 nm was observed at 618.7 nm, corresponding to the zero phonon line of SnV centers in bulk diamond. The Debye–Waller factor for this peak at room temperature was estimated to be 0.38 and so was slightly greater than the value for bulk diamond. A second-order correlation function yielded a g 2 (0) value of 0.04 ± 0.11, indicating single-photon emission. The successful creation of single SnV centers in nanodiamonds is a critical step toward integrating nanophotonic devices for photonic quantum technologies.
Group-IV color centers in diamonds are promising not only as spin-photon interfaces for quantum networks but also as multicolor photoluminescence probes and all-optical temperature sensors for biological research. Therefore, generating group-IV color centers in detonation nanodiamonds (DNDs), the smallest class of diamond nanocrystals, has become a research focal point. This approach holds potential for the noninvasive introduction of diamond sensors into living cell organelles, enabling sensing of local structural and temperature changes with minimal disturbance. Following the successful generation of silicon- and germanium-vacancy centers in DNDs, the generation of tin-vacancy (SnV) centers was investigated. Similar to other group-IV color centers, the SnV centers exhibit strong photoluminescence. In addition, the SnV center offers a long spin coherence time compared with those of silicon- and germanium-vacancy centers. However, the strain induced by large Sn atoms poses substantial challenges for generating SnV centers in ultrasmall nanodiamonds. In this study, Sn-doped DNDs with a mean particle size of ~ 5 nm were subjected to a 3 days boiling acid treatment, which led to sharp zero-phonon lines of SnV centers at ~ 620 nm in the photoluminescence spectra. Photon autocorrelation measurements further revealed the presence of single SnV centers in these DNDs.
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 (~10 3 ) 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.
Fluorescent emitters in diamond are considered to be a valuable resource for fields such as quantum communication, quantum photonics, and biological imaging. In this paper, we report a wide range of narrow bandwidth ( ~ 1.5 nm) spectral emission lines arising from different color centers at room temperature. The defects were created by chemical vapor deposition of thin diamond films grown on silica substrates seeded with nanoparticles of diamond and nickel. These fluorescent lines also possess single or few centers photon statistics. We correlate the zero-phonon lines, observed using confocal microscopy, with previously identified nickel-related centers which have been observed in high-pressure high-temperature diamond, with a Si/Ni complex and silicon vacancy defects. We compare our findings with recent results demonstrating single-photon emission in diamond associated with nickel-related centers to clarify and summarize previous studies concerning this specific dopant. The great variety of emission lines observed in the synthesized material, mainly associated with nickel-related centers, could be an important resource for applications relying on the presence of several emitters of single photons in the same sample. Moreover, the possibility of mass production of these centers in nanodiamonds in colloidal suspension may provide an important resource for biomarking and microscopy.
Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.