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Advanced Quantum Technologies

Bottom‐Up Synthesis of Single Crystal Diamond Pyramids Containing Germanium Vacancy Centers

Milad Nonahal, Simon White, Blake Regan, Chi Li, Aleksandra Trycz, Sejeong Kim, Igor Aharonovich, Mehran Kianinia

Published May 14, 2021• 2 citations
Publisher

Abstract

Abstract Diamond resonators containing color‐centers are highly sought after for application in quantum technologies. Bottom‐up approaches are promising for the generation of single‐crystal diamond structures with purposely introduced color centers. Here the possibility of using a polycrystalline diamond to grow single‐crystal diamond structures by employing a pattern growth method is demonstrated. For, the possible mechanism of growing a single‐crystal structure with predefined shape and size from a polycrystalline substrate by controlling the growth condition is clarified. Then, by introducing germanium impurities during the growth, localized and enhanced emission from fabricated pyramid shaped single‐crystal diamonds containing germanium vacancy (GeV) color centers is demonstrated. Finally, linewidth of ∼500 MHz at 4 K from a single GeV center in the pyramid shaped diamonds is measured. The method is an important step toward fabrication of 3D structures for integrated diamond photonics.

DOI
10.1002/qute.202100037

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Abstract Diamond resonators containing color‐centers are highly sought after for application in quantum technologies. Bottom‐up approaches are promising for the generation of single‐crystal diamond structures with purposely introduced color centers. Here the possibility of using a polycrystalline diamond to grow single‐crystal diamond structures by employing a pattern growth method is demonstrated. For, the possible mechanism of growing a single‐crystal structure with predefined shape and size from a polycrystalline substrate by controlling the growth condition is clarified. Then, by introducing germanium impurities during the growth, localized and enhanced emission from fabricated pyramid shaped single‐crystal diamonds containing germanium vacancy (GeV) color centers is demonstrated. Finally, linewidth of ∼500 MHz at 4 K from a single GeV center in the pyramid shaped diamonds is measured. The method is an important step toward fabrication of 3D structures for integrated diamond photonics.
© 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.
We present a new approach combining top down fabrication and bottom up overgrowth to create diamond photonic nanostructures in the form of single-crystalline diamond nanopyramids. Our approach relies on diamond nanopillars, that are overgrown with single-crystalline diamond to form pyramidal structures oriented along crystal facets. To characterize the photonic properties of the pyramids, color centers are created in a controlled way using ion implantation and annealing. We find very high collection efficiency from color centers close to the pyramid apex. We further show excellent smoothness and sharpness of our diamond pyramids with measured tip radii on the order of 10 nm. Our results offer interesting prospects for nanoscale quantum sensing using diamond color centers, where our diamond pyramids could be used as scanning probes for nanoscale imaging. There, our approach would offer significant advantages compared to the cone-shaped scanning probes which define the current state of the art.
Single-color centers in thin polycrystalline diamond membranes allow the platform to be used in integrated quantum photonics, hybrid quantum systems, and other complex functional materials. While single-crystal diamond membranes are still technologically challenging to fabricate as they cannot be grown on a non-diamond substrate, free-standing polycrystalline diamond membranes can be conveniently fabricated at large-scale from nanocrystalline diamond seeds on a substrate that can be selectively etched. However, their practical application for quantum photonics is so far limited by crystallographic defects, impurities, graphitic grain boundaries, small grain sizes, scattering loss, and strain. In this paper, we report on a single-photon source based on silicon-vacancy color centers in a polycrystalline diamond membrane. We discuss the spectroscopic approach and quantify the photon statistics, obtaining a g2(0) ≈ 0.04. Our findings hold promise for introducing polycrystalline diamond to quantum photonics and hybrid quantum systems.
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.
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 are promising solid-state qubits for scalable quantum photonics applications. Amongst many defects, those with inversion symmetry are of an interest due to their promising optical properties. In this work, we demonstrate a maskless implantation of an array of bright, single germanium vacancy (GeV) centers in diamond. Employing the direct focused ion beam technique, single GeV emitters are engineered with the spatial accuracy of tens of nanometers. The single GeV creation ratio reaches as high as 53% with the dose of 200 Ge + ions per spot. The presented fabrication method is promising for future nanofabrication of integrated photonic structures with GeV emitters as a leading platform for spin-spin interactions.