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ACS Applied Materials & Interfaces

Controlled Doping of GeV and SnV Color Centers in Diamond Using Chemical Vapor Deposition

Mika T. Westerhausen, Aleksandra Trycz, Connor Stewart, Milad Nonahal, Blake Regan, Mehran Kianinia, Igor Aharonovich

Published Jun 3, 2020• 24 citations
Publisher

Abstract

Group IV color centers in diamond (Si, Ge, Sn, and Pb) have recently emerged as promising candidates for realization of scalable quantum photonics. However, their synthesis in nanoscale diamond is still in its infancy. In this work we demonstrate controlled synthesis of selected group IV defects (Ge and Sn) into nanodiamonds and nanoscale single crystal diamond membranes by microwave plasma chemical vapor deposition. We take advantage of inorganic salts to prepare the chemical precursors that contain the required ions that are then incorporated into the growing diamond. Photoluminescence measurements confirm that the selected group IV emitters are present in the diamond without degrading its structural quality. Our results are important to expand the versatile synthesis of color centers in diamond.

DOI
10.1021/acsami.0c07242

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Group IV color centers in diamond (Si, Ge, Sn, and Pb) have recently emerged as promising candidates for realization of scalable quantum photonics. However, their synthesis in nanoscale diamond is still in its infancy. In this work we demonstrate controlled synthesis of selected group IV defects (Ge and Sn) into nanodiamonds and nanoscale single crystal diamond membranes by microwave plasma chemical vapor deposition. We take advantage of inorganic salts to prepare the chemical precursors that contain the required ions that are then incorporated into the growing diamond. Photoluminescence measurements confirm that the selected group IV emitters are present in the diamond without degrading its structural quality. Our results are important to expand the versatile synthesis of color centers in diamond.
Group IV color centers in diamond are promising single-photon emitters for quantum information processing and networking. Among them, the tin-vacancy (SnV) center stands out due to its long spin coherence times at cryogenic temperatures above 1 K. While SnV centers have been realized using various fabrication routes, their in situ formation via microwave plasma-enhanced chemical vapor deposition (MW PE CVD) remains relatively unexplored. In this study, SnV centers, identified by a zero-phonon line (ZPL) near 620 nm, were synthesized in nanocrystalline diamond and free-standing microcrystalline diamond using tin oxide (SnO 2 ) as a dopant source at substrate temperatures of 750°C and 850°C. Photoluminescence measurements reveal that lowering the substrate temperature enhances both the ZPL intensity and spatial uniformity of SnV centers. These results highlight substrate temperature as a key parameter for controlling SnV incorporation during MW PE CVD growth and provide insights into optimizing fabrication strategies for diamond-based quantum technologies.
Group IV color centers in diamond have garnered great interest for their potential as optically active solid-state spin qubits. The future utilization of such emitters requires the development of precise site-controlled emitter generation techniques that are compatible with high-quality nanophotonic devices. This task is more challenging for color centers with large group IV impurity atoms, which are otherwise promising because of their predicted long spin coherence times without a dilution refrigerator. For example, when applied to the negatively charged tin-vacancy (SnV – ) center, conventional site-controlled color center generation methods either damage the diamond surface or yield bulk spectra with unexplained features. Here we demonstrate a novel method to generate site-controlled SnV – centers with clean bulk spectra. We shallowly implant Sn ions through a thin implantation mask and subsequently grow a layer of diamond via chemical vapor deposition. This method can be extended to other color centers and integrated with quantum nanophotonic device fabrication.
Progress in controlling diamond synthesis has made it possible to produce very pure crystals and to incorporate and control atomic impurities and carbon vacancies in the crystal lattice. The appropriate impurity-vacancy combinations can give rise to special defects known as color centers, such as the nitrogen-vacancy (NV) or the silicon-vacancy (SiV), which exhibit exceptional quantum properties with spins that are optically addressable. The use of diamond containing color centers has paved the way for the development of innovative quantum technologies, such as very high-resolution magnetometry and quantum information processing. Nevertheless, the development of quantum sensors at the nanometric scale remains one of the most interesting challenges. In this context, the development of a reliable nanoparticle synthesis technique that allows the desired defects to be incorporated and their quantum optical properties to be modulated is crucial. In this seminar, an efficient and recent method to produce diamond nanoparticles containing NV, SiV and germanium-vacancy (GeV) centers is proposed through direct plasma assisted chemical vapour deposition (CVD) growth. This technique allows good control of both nanoparticle growth processes and color centers formation. The optimization of the CVD nanodiamond growth process is presented, showing the impact of different plasma parameters and gas phasecomposition on nanoparticle crystallinity, size and shape. Morphological characterizations reveal the production of small (around 100 nm) and well faceted nanodiamond particles. In addition, the SiV and GeV color centers incorporation can be tuned within this material by varying the gas phase composition which emphasizes the high flexibility of the CVD growth technique. Finally, the quantum properties of the incorporated color centers have been successfully investigated under extreme pressure conditions (up to ~ 180 GPa) showing a monotonic blue shift of their optical zero-phonon line. Since their luminescence remains stable, SiV and GeV centers emerge as high-pressure nanosensors.
© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement. Color centers in diamond have garnered significant attention for applications in integrated quantum photonics. The availability of thin (~ hundred of nanometers) diamond membranes is paramount to achieve this goal. In this paper, we describe in detail a robust, reproducible and cost effective fabrication method that enables engineering high quality thin diamond membranes with uniform distribution of germanium vacancies employing microwave plasma chemical vapor deposition. We use a combination of different germanium precursors for homogeneous doping of the membranes to increase the probability of germanium incorporation into the diamond lattice. Our fabrication methodology can be further extended to implementation of other color centers in thin diamond membranes and be used for engineering quantum photonic devices.
Group-IV color centers in diamond are promising solid-state quantum emitters due to their favorable optical properties, yet deterministic fabrication via ion implantation remains challenging. We investigated the photoactivation of Si-, Ge-, Sn-, and Pb-implanted diamond using continuous-wave (CW) 405 nm laser irradiation at milliwatt powers. The photoactivation follows a characteristic energy dependence consistent with charge state transitions induced by photon absorption. Notably, the PbV − center demonstrated a photoactivation yield of approximately 0.4%, suggesting a viable route for spatially controlled fabrication of single quantum emitters.
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.