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arXiv:1708.03576 · Physical Review Letters

Tin-Vacancy Quantum Emitters in Diamond

Takayuki Iwasaki, Yoshiyuki Miyamoto, Takashi Taniguchi, Petr Siyushev, Mathias H. Metsch, Fedor Jelezko, Mutsuko Hatano

Published Dec 22, 2017• 324 citations
arXivHTMLPDF

Abstract

Tin-vacancy ($\mathrm{Sn}\text{\ensuremath{-}}V$) color centers were created in diamond via ion implantation and subsequent high-temperature annealing up to $2100\text{ }\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}$ at 7.7 GPa. The first-principles calculation suggested that a large atom of tin can be incorporated into a diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The $\mathrm{Sn}\text{\ensuremath{-}}V$ center showed a sharp zero phonon line at 619 nm at room temperature. This line split into four peaks at cryogenic temperatures, with a larger ground state splitting ($\ensuremath{\sim}850\text{ }\text{ }\mathrm{GHz}$) than that of color centers based on other group-IV elements, i.e., silicon-vacancy ($\mathrm{Si}\text{\ensuremath{-}}V$) and germanium-vacancy ($\mathrm{Ge}\text{\ensuremath{-}}V$) centers. The excited state lifetime was estimated, via Hanbury Brown--Twiss interferometry measurements on single $\mathrm{Sn}\text{\ensuremath{-}}V$ quantum emitters, to be $\ensuremath{\sim}5\text{ }\text{ }\mathrm{ns}$. The order of the experimentally obtained optical transition energies, compared with those of $\mathrm{Si}\text{\ensuremath{-}}V$ and $\mathrm{Ge}\text{\ensuremath{-}}V$ centers, was in good agreement with the theoretical calculations.

DOI
10.1103/physrevlett.119.253601

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Tin-vacancy (Sn\ensuremath-V\mathrm{Sn}\text{\ensuremath{-}}VSn\ensuremath-V) color centers were created in diamond via ion implantation and subsequent high-temperature annealing up to 2100 \ifmmode∘\else\textdegree\fiC2100\text{ }\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}2100 \ifmmode∘\else\textdegree\fiC at 7.7 GPa. The first-principles calculation suggested that a large atom of tin can be incorporated into a diamond lattice with a split-vacancy configuration, in which a tin atom sits on an interstitial site with two neighboring vacancies. The Sn\ensuremath-V\mathrm{Sn}\text{\ensuremath{-}}VSn\ensuremath-V center showed a sharp zero phonon line at 619 nm at room temperature. This line split into four peaks at cryogenic temperatures, with a larger ground state splitting (\ensuremath∼850  GHz\ensuremath{\sim}850\text{ }\text{ }\mathrm{GHz}\ensuremath∼850  GHz) than that of color centers based on other group-IV elements, i.e., silicon-vacancy (Si\ensuremath-V\mathrm{Si}\text{\ensuremath{-}}VSi\ensuremath-V) and germanium-vacancy (Ge\ensuremath-V\mathrm{Ge}\text{\ensuremath{-}}VGe\ensuremath-V) centers. The excited state lifetime was estimated, via Hanbury Brown--Twiss interferometry measurements on single Sn\ensuremath-V\mathrm{Sn}\text{\ensuremath{-}}VSn\ensuremath-V quantum emitters, to be \ensuremath∼5  ns\ensuremath{\sim}5\text{ }\text{ }\mathrm{ns}\ensuremath∼5  ns. The order of the experimentally obtained optical transition energies, compared with those of Si\ensuremath-V\mathrm{Si}\text{\ensuremath{-}}VSi\ensuremath-V and Ge\ensuremath-V\mathrm{Ge}\text{\ensuremath{-}}VGe\ensuremath-V centers, was in good agreement with the theoretical calculations.
Quantum emitters in diamond are a promising candidate for quantum network applications. Here, we show basic properties of tin-vacancy (SnV) centers in diamond, which we recently discovered. The SnV center shows a sharp zero phonon line and a high fluorescence intensity. The SnV center has a possibility to have a long spin coherence time in the Kelvin temperature range, in contrast to other group-IV color centers, i.e. silicon-vacancy and germanium-vacancy centers. We discuss important experiments regarding spin and optical properties of the SnV quantum emitter for further development towards quantum network.
Nanodiamonds containing single tin-vacancy (SnV) centers have the potential for integration into nanophotonic devices employed in quantum technologies such as quantum sensing, quantum information processing and quantum communication. The present study assessed single SnV centers in nanodiamonds less than 10 nm in size. Such centers were generated by implanting Sn ions into size-selected small nanodiamonds followed by high-temperature annealing. A sharp emission peak with a line width of 2.6 nm was observed at 618.7 nm, corresponding to the zero phonon line of SnV centers in bulk diamond. The Debye–Waller factor for this peak at room temperature was estimated to be 0.38 and so was slightly greater than the value for bulk diamond. A second-order correlation function yielded a g 2 (0) value of 0.04 ± 0.11, indicating single-photon emission. The successful creation of single SnV centers in nanodiamonds is a critical step toward integrating nanophotonic devices for photonic quantum technologies.
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.
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.
Color centers in diamond have attracted much interest as candidates for optically active, solid-state quantum bits. Of particular interest are inversion-symmetric color centers based on group-IV impurities in diamond because they emit strongly into their zero-phonon lines and are insensitive to electric field noise to first order. Early studies of the negatively charged tin-vacancy (${\mathrm{SnV}}^{\ensuremath{-}}$) center in diamond have found the ${\mathrm{SnV}}^{\ensuremath{-}}$ to be a promising candidate: it has high quantum efficiency, emits strongly into its zero-phonon lines, and is expected to have a long T2{T}_{2}T2​ spin coherence time at 4 K. To develop the ${\mathrm{SnV}}^{\ensuremath{-}}$ into a spin qubit requires further characterization, especially of the spin and optical properties of individual ${\mathrm{SnV}}^{\ensuremath{-}}$ in nanofabricated structures. In this work, we isolate single ${\mathrm{SnV}}^{\ensuremath{-}}$ centers in diamond nanopillars and characterize their emission properties and their spin response to a magnetic field. We observe narrow emission linewidths <250<250<250 MHz, as well as a strong polarization dependence of each transition. We also find the Zeeman splitting under a magnetic field to be in good agreement with theoretical prediction. Our results pave the way toward future employment of single ${\mathrm{SnV}}^{\ensuremath{-}}$ centers as optically accessible quantum memories.