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Nano Letters

Two-Level Ultrabright Single Photon Emission from Diamond Nanocrystals

Igor Aharonovich, Stefania Castelletto, David Simpson, Alastair D. Stacey, Jeffrey Colin McCallum, Andrew D. Greentree, Steven Prawer

Published Aug 11, 2009• 136 citations
Publisher

Abstract

The fabrication of stable ultrabright single photon sources operating at room temperature is reported. The emitter is based on a color center within a diamond nanocrystal grown on a sapphire substrate by chemical vapor deposition method and exhibits a two-level electronic behavior with a maximum measured count rate of 3.2 x 10(6) counts/s at saturation. The emission is centered at approximately 756 nm with a full width at half-maximum approximately 11 nm and an excited state lifetime of 3.7 ns. These unique properties make it a leading candidate for quantum photonics and communication applications as well as for cellular biomarking.

DOI
10.1021/nl9014167

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The fabrication of stable ultrabright single photon sources operating at room temperature is reported. The emitter is based on a color center within a diamond nanocrystal grown on a sapphire substrate by chemical vapor deposition method and exhibits a two-level electronic behavior with a maximum measured count rate of 3.2 x 10(6) counts/s at saturation. The emission is centered at approximately 756 nm with a full width at half-maximum approximately 11 nm and an excited state lifetime of 3.7 ns. These unique properties make it a leading candidate for quantum photonics and communication applications as well as for cellular biomarking.
Quantum communication and quantum metrology established a demand for an accessible solid state systems which can generate a stream of single photons on demand [1]. Although single photon emission has been demonstrated from quantum dots (QD)[1,2], single molecules [3] and nanowires [4], their practical operation is limited by the temperature or photostability. Diamond crystals, however, are the most promising platform for generation of robust, photo-stable, single photons at room temperature [5,6]. Nevertheless, out of more than 500 existing optical centers in diamond only three known centers demonstrated a clear single photon emission: the nitrogen-vacancy complex [6,7], the silicon-vacancy complex [8] and the nickel-nitrogen complex [9,10]. Recent progress in materials science and fabrication techniques of diamond color centers unveiled novel quantum emitters with photo-physical properties surpassing the current mainstream [11,12,13]. Consequently, the versatility of the diamond lattice to host various impurities which give luminescence signals lead to a dramatic discovery of ultra bright single photon emitters operating in the MHz regime [14]. These new centers, comparable with QD in terms of brightness [1], but have the tremendous advantage of their room temperature operation and photo-stability. Furthermore, it opened a new avenue to investigate essentially an unknown group of single photon emitters. A brief description of the fabrication methods and a detailed quantum optical characterization of this class of diamond emitters is the subject of this presentation. In particular we will present the photo-physical properties of a novel family of single photon emitters, most likely originated from Cr impurities within the chemical vapor deposition grown nano-diamond crystals. We concentrate on the typical emission lines in the range of 740 - 790 nm, which exhibit single photon emission with count rate in the range of 0.8-3.2 106 counts/s at the limit of infinite optical excitation power, and life time as short as 1 ns. Even more, some of the emitters exhibit a photon statistics without any photon bunching, indicating a two-level system with unitary quantum efficiency. We will also show preliminary results of a resonant excitation at 4 K. We will highlight future directions to optimize these sources and avenues to investigate the fundamental properties of these centers.
A detailed study of the photophysical properties of several chromium-related color centers produced within chemical vapor deposition diamond is presented. These emitters show narrow luminescence lines in the range of $740\ensuremath{-}770$ nm. Single-photon emission was verified with continuous and pulsed excitation with detected emission rates at saturation in the range of ($2\ensuremath{-}3$) $\ifmmode\times\else\texttimes\fi{}$ 106{10}^{6}106 counts/s, while direct lifetime measurements reveal excited state lifetimes for the distinct centers ranging $1\ensuremath{-}14$ ns. In addition, a number of quantum emitters demonstrate two-level behavior with no bunching present in the second-order correlation function. The three-level systems revealed typically photoluminescence lines with width half-maximum of  4~4 4 nm while the two-level emitters have full width half-maximum of  10~10 10 nm at room temperature. In addition, the quantum efficiency of the two-level system was measured to be four times higher than that of the three-level system.
Color centers in diamond are very promising candidates among the possible realizations for practical singlephoton sources because of their long-time stable emission at room temperature. The popular nitrogen-vacancy center shows single-photon emission, but within a large, phonon-broadened spectrum (≈ 100 nm), which strongly limits its applicability for quantum communication. By contrast, Ni-related centers exhibit narrow emission lines at room temperature. We present investigations on single color centers consisting of Ni and Si created by ion implantation into single crystalline IIa diamond. We use systematic variations of ion doses between 108 cm-2 and 1014 cm-2 and energies between 30 keV and 1.8MeV. The Ni-related centers show emission in the near infrared spectral range (≈ 770 nm to 787 nm) with a small line-width (≈ 3 nm FWHM). A measurement of the intensity correlation function proves single-photon emission. Saturation measurements yield a rather high saturation count rate of 77.9kcounts/s. Polarization dependent measurements indicate the presence of two orthogonal dipoles.
Quantum information processing and integrated nanophotonics require robust generation of single photon emitters on demand. In this work, we demonstrate that diamond films grown on a silicon substrate by microwave plasma chemical vapor deposition can host bright, narrowband single photon emitters in the visible—near infra-red spectral range. The emitters possess fast lifetime (∼several ns), absolute photostability, and exhibit full polarization at excitation and emission. Pulsed and continuous laser excitations confirm their quantum behaviour at room temperature, while low temperature spectroscopy is performed to investigate inhomogeneous broadening. Our results advance the knowledge of solid state single photon sources and open pathways for their practical implementation in quantum communication and quantum information processing.