Carbon trimer as a 2 eV single-photon emitter candidate in hexagonal boron nitride: A first-principles study

Journal Article · 29 April 2022 · Physical Review Materials

DOI: https://doi.org/10.1103/physrevmaterials.6.l042201 · OSTI ID:1889529

Li, Kejun  ^[1]; Smart, Tyler J. ^[2]; Ping, Yuan  ^[1]

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1. Univ. of California, Santa Cruz, CA (United States)
2. Univ. of California, Santa Cruz, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

The generation of single-photon emitters in hexagonal boron nitride around 2 eV emission is experimentally well recognized; however, the atomic nature of these emitters is unknown. In this Letter, we use first-principles calculations to demonstrate that carbon trimer substitutional defect (C₂C_N) is a possible source of 2 eV single-photon emitter in hBN. Here, we showcase the calculations of a complete set of static and dynamical properties related to quantum defects, including exciton-defect couplings and electron-phonon interactions, from both density functional theory and many-body perturbation theory. In particular, we show that it is critical to consider both radiative and nonradiative processes when comparing with experimental lifetime for known 2 eV emitters. We find that C₂C_N has several key physical properties matching the ones of experimentally observed single-photon emitters. These include the zero-phonon line (2.13 eV), Huang-Rhys factor (1.35), photoluminescence lifetime (2.19 ns), phonon-sideband energy (180 meV), and photoluminescence spectrum. The identification of defect candidates for 2 eV emission paves the way for controllable single-photon emission generation.

• Research Organization: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
• Sponsoring Organization: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
• Grant/Contract Number: AC52-07NA27344; DMR-1760260; SC0012704; AST 1828315; AC02-05CH11231; ACI-1548562; LDRD 20-SI-004
• OSTI ID: 1889529
• Alternate ID(s): OSTI ID: 1892117
• Report Number(s): LLNL-JRNL-840246; 1061438; TRN: US2310056
• Journal Information: Physical Review Materials, Vol. 6, Issue 4; ISSN 2475-9953
• Publisher: American Physical Society (APS)Copyright Statement
• Country of Publication: United States
• Language: English