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arXiv:1805.12202 · Physical review. B./Physical review. B

Lead-related quantum emitters in diamond

Matthew E. Trusheim, Noel Wan, Kevin C. Chen, Christopher J. Ciccarino, Johannes Flick, Ravishankar Sundararaman, Girish Malladi, Eric A. Bersin, Michael E. Walsh, Benjamin Lienhard, H. Bakhru, Prineha Narang, Dirk Englund

Published Feb 21, 2019• 122 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevb.99.075430

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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.
We report the optical observation of lead-vacancy (PbV) centers in diamond fabricated by Pb ion implantation and subsequent high-temperature annealing (2100 °C) under high pressure (7.7 GPa). Their optical properties were characterized by photoluminescence at varying temperatures down to 5.7 K. We observed intense emission peaks at 550 and 554 nm, with a large splitting of approximately 3900 GHz. The two lines are thought to correspond to the zero phonon line (ZPL) of PbV centers with split ground and excited states. A cubic trend of the ZPL width was observed while varying the temperature. We performed polarization measurements of the two lines in a single PbV center, showing nearly orthogonal dipole polarizations. These optical measurements strongly indicate that the PbV center possesses D 3 d symmetry in the diamond lattice. The observed large ground state splitting significantly suppresses the phonon-mediated transition, which causes decoherence of the electron spin state of the group IV color centers in diamond, leading to the expectation of a long spin coherence time at a temperature ∼9 K.
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.
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.
Transform-limited photon emission from quantum emitters is essential for high-fidelity entanglement generation. In this Letter, we report the coherent optical property of a single negatively charged lead-vacancy (PbV) center in diamond. Photoluminescence excitation measurements reveal stable fluorescence with a linewidth of 39 MHz at 6 K, close to the transform limit estimated from the lifetime measurement. We observe 4 orders of magnitude different linewidths of the two zero-phonon lines, and find that the phonon-induced relaxation in the ground state contributes to this huge difference in the linewidth. Because of the suppressed phonon absorption in the PbV center, we observe nearly transform-limited photon emission up to 16 K, demonstrating its high temperature robustness compared to other color centers in diamond.
A negatively charged lead-vacancy (PbV-) center in diamond is a novel quantum system which can be operated at a high temperature above 4 K owing to its large ground state splitting. To unlock the quantum properties of the PbV- center, the enhancement of the fluorescence intensity is a key issue. Here, we demonstrate enhanced emission from PbV- centers by a factor of approximately 10 using solid immersion lenses (SILs) fabricated on rough diamond surface caused by high-temperature anneal over 2000°C. Resonant excitation reveals the narrow emission close to the transform-limited linewidth. Furthermore, we demonstrate two-photon interference using one single PbV- center in an SIL. This enhanced emission and indistinguishability will lead to further development of the PbV- center towards quantum network node applications.