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arXiv:1806.01608 · ACS Photonics

Single-Photon Emitters in Lead-Implanted Single-Crystal Diamond

Sviatoslav Ditalia Tchernij, Tobias Lühmann, Tobias Herzig, Johannes Küpper, Alessandro Damin, S. Santonocito, Matteo Signorile, P. Traina, Ekaterina V. Moreva, Federica Celegato, Sébastien Pezzagna, Ivo Pietro Degiovanni, P. Olivero, M. Jakšić, Jan Meijer, Marco Genovese, J. Forneris

Published Nov 12, 2018• 101 citations

Abstract

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.

DOI: 10.1021/acsphotonics.8b01013

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Abstract We report on the systematic characterization of the optical properties of diamond color centers based on Pb impurities. An ensemble photoluminescence analysis of their spectral emission was performed at different excitation wavelengths in the 405–520 nm range and at different temperatures in the 4–300 K range. The series of observed spectral features consist of different emission lines associated with Pb-related defects. Finally, a room-temperature investigation of single-photon emitters under 490.5 nm laser excitation is reported, revealing different spectral signatures with respect to those already reported under 514 nm excitation. This work represents a substantial progress with respect to previous studies on Pb-related color centers, both in the attribution of an articulated series of spectral features and in the understanding of the formation process of this type of defect, thus clarifying the potential of this system for high-impact applications in 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 diamond are promising solid-state quantum emitters due to their favorable optical properties, yet deterministic fabrication via ion implantation remains challenging. We investigated the photoactivation of Si-, Ge-, Sn-, and Pb-implanted diamond using continuous-wave (CW) 405 nm laser irradiation at milliwatt powers. The photoactivation follows a characteristic energy dependence consistent with charge state transitions induced by photon absorption. Notably, the PbV − center demonstrated a photoactivation yield of approximately 0.4%, suggesting a viable route for spatially controlled fabrication of single quantum emitters.

Diamond is a promising platform for the development of technological applications in quantum optics and photonics. The quest for color centers with optimal photo-physical properties has led in recent years to the search for novel impurity-related defects in this material. Here, we report on a systematic investigation of the photo-physical properties of two He-related (HR) emission lines at 535.2 nm and 559.7 nm (as measured at a temperature of 25 K) created in three different diamond substrates upon implantation with 1.3 MeV He+ ions and subsequent annealing. The spectral features of the HR centers were studied in an “optical grade” diamond substrate as a function of several physical parameters, namely, the measurement temperature, the excitation wavelength, and the intensity of external electric fields. The emission lifetimes of the 535.2 nm and 559.7 nm lines were also measured by means of time-gated photoluminescence measurements. The Stark shifting of the HR centers under the application of an external electrical field was observed in a CVD diamond film equipped with buried graphitic electrodes, suggesting the lack of inversion symmetry in the defects' structure. Furthermore, the photoluminescence mapping under 405 nm excitation of a “detector grade” diamond sample implanted at a He+ ion fluence of 1 × 1010 cm−2 enabled us to identify the spectral features of both the HR emission lines from the same localized optical spots. The reported results provide an insight into the structure of He-related defects in diamond and their possible utilization in practical applications.

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.