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arXiv:2010.15475 · AVS Quantum Science

Single germanium vacancy centers in nanodiamonds with bulk-like spectral stability

Mackrine Nahra, Daniel Alshamaa, Régis Déturche, Валерий Александрович Давыдов, L. F. Kulikova, V. Agafonov, Christophe Couteau

Published Jan 29, 2021• 30 citations
arXivHTMLPDF

Abstract

Motivated by the success of group IV color centers in nanodiamonds (NDs) for hybrid technology requiring a single photon source, the authors study single germanium-vacancy (GeV−) centers in NDs at room temperature with size ranging from 10 to 50 nm and with remarkable spectral properties. The authors characterize their zero-phonon line, study their internal population dynamics, and compare their emission properties in the framework of a three level model with intensity dependent de-shelving. Furthermore, the authors characterize their lifetime, polarization, and brightness. The authors find a maximum photon emission count rate of 1.6 MHz at saturation. The authors also report a polarization visibility of 92% from the fluorescence light, which potentially makes GeV− centers good candidates for quantum key distribution requiring polarized single photons. The authors show that GeV− centers in NDs presented in this work have a comparable spectral stability compared to their bulk counterpart, which is needed for future applications using nanodiamonds.

DOI
10.1116/5.0035937

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Motivated by the success of group IV color centers in nanodiamonds (NDs) for hybrid technology requiring a single photon source, the authors study single germanium-vacancy (GeV−) centers in NDs at room temperature with size ranging from 10 to 50 nm and with remarkable spectral properties. The authors characterize their zero-phonon line, study their internal population dynamics, and compare their emission properties in the framework of a three level model with intensity dependent de-shelving. Furthermore, the authors characterize their lifetime, polarization, and brightness. The authors find a maximum photon emission count rate of 1.6 MHz at saturation. The authors also report a polarization visibility of 92% from the fluorescence light, which potentially makes GeV− centers good candidates for quantum key distribution requiring polarized single photons. The authors show that GeV− centers in NDs presented in this work have a comparable spectral stability compared to their bulk counterpart, which is needed for future applications using nanodiamonds.
Atomic-sized fluorescent defects in diamond are widely recognized as a promising solid state platform for quantum cryptography and quantum information processing. For these applications, single photon sources with a high intensity and reproducible fabrication methods are required. In this study, we report a novel color center in diamond, composed of a germanium (Ge) and a vacancy (V) and named the GeV center, which has a sharp and strong photoluminescence band with a zero-phonon line at 602 nm at room temperature. We demonstrate this new color center works as a single photon source. Both ion implantation and chemical vapor deposition techniques enabled fabrication of GeV centers in diamond. A first-principles calculation revealed the atomic crystal structure and energy levels of the GeV center.
Color centers in diamond—especially group IV defects—have been advanced as a viable solid-state platform for quantum photonics and information technologies. We investigate the photodynamics and characteristics of germanium-vacancy (GeV) centers hosted in high-pressure high-temperature diamond nanocrystals. Through back-focal plane imaging, we analyze the far-field radiation pattern of the investigated emitters and derive a crossed-dipole emission, which is strongly aligned along one axis. We use this information in combination with lifetime measurements to extract the decay rate statistics of the GeV emitters and determine their quantum efficiency, which we estimated to be ∼ ( 22 ± 2 ) % . Our results offer further insight into the photodynamic properties of the GeV center in nanodiamonds and confirm its suitability as a desirable system for quantum technologies.
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.
The development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.