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Physical Review Letters

Direct Structural Identification and Quantification of the Split-Vacancy Configuration for Implanted Sn in Diamond

Ulrich Wahl, J. G. Correia, Renán Villarreal, Emilie Bourgeois, Michal Gulka, Miloš Nesládek, A. Vantomme, L. M. C. Pereira

Published Jul 22, 2020• 29 citations
Publisher

Abstract

We demonstrate formation of the ideal split-vacancy configuration of the Sn-vacancy center upon implantation into natural diamond. Using ${\ensuremath{\beta}}^{\ensuremath{-}}$ emission channeling following low fluence $^{121}\mathrm{Sn}$ implantation ($2\ifmmode\times\else\texttimes\fi{}{10}^{12}\text{ }\text{ }\mathrm{atoms}/{\mathrm{cm}}^{2}$, 60 keV) at the ISOLDE facility at CERN, we directly identified and quantified the atomic configurations of the Sn-related centers. Our data show that the split-vacancy configuration is formed immediately upon implantation with a surprisingly high efficiency of $\ensuremath{\approx}40%$. Upon thermal annealing at $920\text{ }\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}$ $\ensuremath{\approx}30%$ of Sn is found in the ideal bond-center position. Photoluminescence revealed the characteristic $\mathrm{Sn}{V}^{\ensuremath{-}}$ line at 621 nm, with an extraordinarily narrow ensemble linewidth (2.3 nm) of near-perfect Lorentzian shape. These findings further establish the $\mathrm{Sn}{V}^{\ensuremath{-}}$ center as a promising candidate for single photon emission applications, since, in addition to exceptional optical properties, it also shows a remarkably simple structural formation mechanism.

DOI
10.1103/physrevlett.125.045301

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We demonstrate formation of the ideal split-vacancy configuration of the Sn-vacancy center upon implantation into natural diamond. Using \ensuremathβ\ensuremath−{\ensuremath{\beta}}^{\ensuremath{-}}\ensuremathβ\ensuremath− emission channeling following low fluence 121Sn^{121}\mathrm{Sn}121Sn implantation (2\ifmmode×\else\texttimes\fi1012  atoms/cm22\ifmmode\times\else\texttimes\fi{}{10}^{12}\text{ }\text{ }\mathrm{atoms}/{\mathrm{cm}}^{2}2\ifmmode×\else\texttimes\fi1012  atoms/cm2, 60 keV) at the ISOLDE facility at CERN, we directly identified and quantified the atomic configurations of the Sn-related centers. Our data show that the split-vacancy configuration is formed immediately upon implantation with a surprisingly high efficiency of \ensuremath≈40\ensuremath{\approx}40%\ensuremath≈40. Upon thermal annealing at 920 \ifmmode∘\else\textdegree\fiC920\text{ }\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}920 \ifmmode∘\else\textdegree\fiC \ensuremath≈30\ensuremath{\approx}30%\ensuremath≈30 of Sn is found in the ideal bond-center position. Photoluminescence revealed the characteristic SnV\ensuremath−\mathrm{Sn}{V}^{\ensuremath{-}}SnV\ensuremath− line at 621 nm, with an extraordinarily narrow ensemble linewidth (2.3 nm) of near-perfect Lorentzian shape. These findings further establish the SnV\ensuremath−\mathrm{Sn}{V}^{\ensuremath{-}}SnV\ensuremath− center as a promising candidate for single photon emission applications, since, in addition to exceptional optical properties, it also shows a remarkably simple structural formation mechanism.
We provide the first systematic characterization of the structural and photoluminescence properties of optically active centers fabricated upon implantation of 30–100 keV Mg + ions in synthetic diamond. The structural configurations of Mg-related defects were studied by the electron emission channeling technique for short-lived, radioactive 27 Mg implantations at the CERN-ISOLDE facility, performed both at room temperature and 800 °C, which allowed the identification of a major fraction of Mg atoms (∼30 to 42%) in sites which are compatible with the split-vacancy structure of the MgV complex. A smaller fraction of Mg atoms (∼13 to 17%) was found on substitutional sites. The photoluminescence emission was investigated both at the ensemble and individual defect level in the 5–300 K temperature range, offering a detailed picture of the MgV-related emission properties and revealing the occurrence of previously unreported spectral features. The optical excitability of the MgV center was also studied as a function of the optical excitation wavelength to identify the optimal conditions for photostable and intense emission. The results are discussed in the context of the preliminary experimental data and the theoretical models available in the literature, with appealing perspectives for the utilization of the tunable properties of the MgV center for quantum information processing applications.
The fabrication of luminescent defects in single-crystal diamond upon Sn implantation and annealing is reported. The relevant spectral features of the optical centers (emission peaks at 593.5, 620.3, 630.7, and 646.7 nm) are attributed to Sn-related defects through the correlation of their photoluminescence (PL) intensity with the implantation fluence. Single Sn-related defects were identified and characterized through the acquisition of their second-order autocorrelation emission functions, by means of Hanbury-Brown and Twiss interferometry. The investigation of their single-photon emission regime as a function of excitation laser power revealed that Sn-related defects are based on three-level systems with a 6 ns radiative decay lifetime. In a fraction of the studied centers, the observation of a blinking PL emission is indicative of the existence of a dark state. Furthermore, absorption dependence on the polarization of the excitation radiation with ∼45% contrast was measured. This work shed light on the existence of a new optical center associated with a group-IV impurity in diamond, with similar photophysical properties to the already well-known Si–V and Ge–V emitters, thus, providing results of interest from both the fundamental and applicative points of view.
Abstract We report on the creation and characterization of Pb-related color centers in diamond upon ion implantation and subsequent thermal annealing. Their optical emission in the photoluminescence (PL) regime consists of an articulated spectrum with intense emission peaks at 552.1 and 556.8 nm, accompanied by a set of additional lines in the 535–700 nm range. The attribution of the PL emission to stable Pb-based defects is corroborated by the correlation of its intensity with the implantation fluence of Pb ions. PL measurements performed as a function of sample temperature (in the 143–300 K range) and under different excitation wavelengths (i.e., 532, 514, 405 nm) suggest that the complex spectral features observed in Pb-implanted diamond might be related to a variety of different defects and/or charge states. The emission of the 552.1 and 556.8 nm lines is reported at the single-photon emitter level, demonstrating that they originate from the same individual defect. This work follows from previous reports on optically active centers in diamond based on group-IV impurities, such as Si, Ge, and Sn. In perspective, a comprehensive study of this set of defect complexes could bring significant insight on the common features involved in their formation and opto-physical properties, thus offering a basis for the development of a new generation of quantum-optical devices.
Nitrogen-vacancy (NV) centers in diamond with coherent optical transitions are a promising candidate for quantum science and technology protocols. A widely used strategy for their creation is nitrogen-ion implantation and high-temperature annealing. The data presented in this work show that while low-strain, narrow-optical-linewidth NV centers are formed from naturally occurring 14{}^{14}14N atoms, NV centers formed from the implanted 15{}^{15}15N atoms show broadened optical transitions and experience higher strain. These results have immediate implications for the positioning accuracy of current NV center creation protocols.
Tin-vacancy (Sn-VVV) centers in diamond, which possess good optical and spin properties, are a promising system for constructing quantum network nodes. Tin atoms are heavy, though, and generating photons with identical wavelength and linewidth from multiple Sn-VVV emitters is challenging, due to the strain in the diamond host material. This study shows that multiple Sn-VVV centers, formed deep within bulk diamond by ion implantation and high-temperature annealing, emit nearly identical photons. This leads to two-photon interference from distant centers, an important step toward building quantum network nodes.
We report on quantum emission from Pb-related color centers in diamond following ion implantation and high-temperature vacuum annealing. First-principles calculations predict a negatively charged Pb-vacancy (PbV) center in a split-vacancy configuration, with a zero-phonon transition around 2.4 eV. Cryogenic photoluminescence measurements performed on emitters in nanofabricated pillars reveal several transitions, including a prominent doublet near 520 nm. The splitting of this doublet, 5.7 THz, exceeds that reported for other group-IV centers. These observations are consistent with the PbV center, which is expected to have a combination of narrow optical transitions and stable spin states, making it a promising system for quantum network nodes.