Lead-related quantum emitters in diamond

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

Phys. Rev. B 99, 075430 – Published 21 February 2019

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.

Received 7 June 2018
Revised 23 October 2018

DOI:https://doi.org/10.1103/PhysRevB.99.075430

Physics Subject Headings (PhySH)

Atomic orbital Density functional theory Electronic structure of atoms & molecules Photoemission Quantum memories Quantum repeaters Single- and few-photon ionization & excitation

Atomic, Molecular & OpticalQuantum Information, Science & Technology

Authors & Affiliations

Matthew E. Trusheim^1,*, Noel H. Wan¹, Kevin C. Chen¹, Christopher J. Ciccarino^2,3, Johannes Flick², Ravishankar Sundararaman⁴, Girish Malladi⁵, Eric Bersin¹, Michael Walsh¹, Benjamin Lienhard¹, Hassaram Bakhru⁵, Prineha Narang², and Dirk Englund¹

¹Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
²John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
³Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA
⁴Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, New York 12180, USA
⁵College of Nanoscale Science and Engineering, State University of New York Polytechnic Institute, 257 Fuller Road, Albany, New York 12203, USA

^*mtrush@mit.edu

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Issue

Vol. 99, Iss. 7 — 15 February 2019

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Images

Figure 1
PbV calculations from first principles. (a) A Pb atom (black) in a split-vacancy configuration within the diamond lattice (blue spheres: carbon atoms). (b) The electron orbital structure of the PbV defect in a negative charge state. Both the $e_{u}$ and $e_{g}$ orbitals are split as a result of strong spin-orbit coupling. The energy difference between the $e_{u}$ and $e_{g}$ orbitals has been adjusted by the HSE-calculated ZPL energy. (c) The same PbV orbital structure from a hole perspective. (d) Comparison of predicted optical transition energies of group-IV defects with experimental data [18, 20, 21] and the present paper. (e, f) Electron density associated with the negatively charged PbV viewed from the [111] and [110] axes, respectively. The density is primarily distributed to the six nearby carbon atoms of the diamond lattice.
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Figure 2
Calculated relative emission intensity from first principles. Dipole matrix elements between each PbV orbital are calculated and compared for different temperatures using jdftx. (a) Predicted emission at zero temperature. The emitting transitions originate from the lower-energy $e_{u}$ orbital (i.e., channels D and C), under the assumption that thermal equilibrium is achieved prior to emission [30]. In the high-temperature limit presented in panel (b), transitions to all four orbitals are thermodynamically allowed, resulting in a four-peak structure. Filled peaks indicate emission polarized along the PbV [111] direction (transitions B and C), while unfilled peaks are polarized perpendicular to the defect axis. We note that the energy values are corrected according to the HSE-calculated ZPL energy.
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Figure 3
Sample preparation. (a) Simulated Pb ion probability distribution, centered around 58 ± 8 nm in depth. (b) Field profile of an emitter in a nanopillar with a diameter of 225 nm and height of 600 nm. Red arrow: polarization of a dipole emitter. Dashed white line: predicted depth of Pb-related emitters. (c) Scanning electron micrograph of the fabricated nanopillar array. Scale bar: 1 $μ m$ .
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Figure 4
Cryogenic (4 K) emitter characterization. (a) Confocal scan of Pb-related emitters in nanopillars. Colorbar: counts per second. White box: a single emitter of interest as described below. (b) Emission spectrum of the boxed emitter. Four regions with observed emission lines are shaded and labeled. Inset: Antibunched emission with $g^{2} (0) = 0.52$ [ $g^{2} (0) = 0.28$ after background correction] and an antibunching time constant of 3.0 ns. (c) Summary of photoluminescence spectra from 129 pillars. Circles indicate the center of an observed emission peak, and colors correspond to individual pillars horizontally across spectral regions. Top: Histogram of emission peak locations. (d) Overall and conditional probabilities for the observation of emission in each region.
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