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Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences

Narrowband photoluminescence of Tin-Vacancy colour centres in Sn-doped chemical vapour deposition diamond microcrystals

Vadim Sedov, Мартьянов Артём Константинович, Arthur Yu. Neliubov, Ivan A. Tiazhelov, Sergey S. Savin, Ivan Yu. Eremchev, Maksim Eremchev, Margarita Pavlenko, Soumen Mandal, Victor Ralchenko, А. В. Наумов

Published Dec 3, 2023• 12 citations

Abstract

Tin-Vacancy (Sn-V) colour centres in diamond have a spin coherence time in the millisecond range at temperatures of 2 K, so they are promising to be used in diamond-based quantum optical devices. However, the incorporation of large Sn atoms into a dense diamond lattice is a non-trivial problem. The objective of our work is to use microwave plasma-assisted chemical vapour deposition (CVD) to grow Sn-doped diamond with submicron SnO 2 particles as a solid-state source of impurity. Well-faceted diamond microcrystals with sizes of a few micrometres were formed on AlN substrates. The photoluminescence (PL) signal with zero-phonon line (ZPL) peak for Sn-V centre at ≈620 nm was measured at room temperature (RT) and at 7 K. The peak width (full width at half-maximum) was measured to be 1.1–1.7 nm at RT and ≈0.05 nm at 7 K. The observed variations of ZPL shape and position, in particular, narrowing of PL peak at RT and formation of single-line fine structure at low- T , are attributed to strain in the crystallites. The diamond doping with Sn via CVD process offers a new route to from Sn-V colour centre in the bulk of the diamond crystallites. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.

DOI: 10.1098/rsta.2023.0167

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We introduce a process for the fabrication of high-quality, spatially isolated nano-diamonds on iridium via microwave-plasma-assisted chemical vapour deposition (CVD) growth. We perform spectroscopy of single silicon-vacancy (SiV) centres produced during the growth of the nano-diamonds. The colour centres exhibit extraordinary narrow zero-phonon-lines down to 0.7 nm at room temperature. Single photon count rates up to 4.8 Mcps at saturation make these SiV centres the brightest diamond-based single photon sources to date. We measure for the first time the fine structure of a single SiV centre, thus confirming the atomic composition of the investigated colour centres.

Abstract Diamond hosts a wide variety of colour centres that have demonstrated outstanding optical and spin properties. Among them, the nitrogen-vacancy (NV) centre is by far the most investigated owing to its superior characteristics, which promise the development of highly sophisticated quantum devices, in particular for sensing applications. Nevertheless, harnessing the potential of these centres mainly relies on the availability of high quality and purity diamond single crystals that need to be specially designed and engineered for this purpose. Plasma assisted chemical vapour deposition (CVD) has become a key enabling technology in this field of research. Nitrogen can indeed be directly doped in situ into a high crystalline quality diamond matrix in a controlled way, allowing the production of single isolated centres or ensembles that can potentially be integrated into a device. In this paper we will provide an overview of the requirements for synthesizing ‘quantum-grade’ diamond films using CVD. These include the reduction of impurities and surrounding spins that limit coherence times, the control of NV density in a wide range of concentrations as well as their spatial localization within the diamond. Enhancing the charge state and preferential orientation of the colour centres is also discussed. These improvements in material fabrication have contributed to positioning diamond as one of the most promising solid-state quantum systems and the first industrial applications in sensing are just starting to emerge.

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Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.

We study single silicon vacancy (SiV) centres in chemical vapour deposition (CVD) nanodiamonds on iridium as well as an ensemble of SiV centres in a high-quality, low-stress CVD diamond film by using temperature-dependent luminescence spectroscopy in the temperature range 5–295 K. We investigate in detail the temperature-dependent fine structure of the zero-phonon line (ZPL) of the SiV centres. The ZPL transition is affected by inhomogeneous as well as temperature-dependent homogeneous broadening and blue shifts by about 20 cm −1 upon cooling from room temperature to 5 K. We employ excitation power-dependent g (2) measurements to explore the temperature-dependent internal population dynamics of single SiV centres and infer mostly temperature-independent dynamics.