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Elementary excitations of single-photon emitters in hexagonal Boron Nitride (2402.09678v1)

Published 15 Feb 2024 in cond-mat.mes-hall and cond-mat.mtrl-sci

Abstract: Single-photon emitters serve as building blocks for many emerging concepts in quantum photonics. The recent identification of bright, tunable, and stable emitters in hexagonal boron nitride (hBN) has opened the door to quantum platforms operating across the infrared to ultraviolet spectrum. While it is widely acknowledged that defects are responsible for single-photon emitters in hBN, crucial details regarding their origin, electronic levels, and orbital involvement remain unknown. Here, we employ a combination of resonant inelastic X-ray scattering and photoluminescence spectroscopy in defective hBN unveiling an elementary excitation at 285 meV that gives rise to a plethora of harmonics correlated with single-photon emitters. We discuss the importance of N $\pi*$ antibonding orbitals in shaping the electronic states of the emitters. The discovery of the elementary excitations of hBN provides new fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.

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References (49)
  1. Caldwell, J. D. et al. Photonics with hexagonal boron nitride. Nature Reviews Materials 4, 552–567 (2019). URL https://www.nature.com/articles/s41578-019-0124-1. Number: 8 Publisher: Nature Publishing Group.
  2. Quantum emission from hexagonal boron nitride monolayers. Nature Nanotechnology 11, 37–41 (2016). URL https://www.nature.com/articles/nnano.2015.242. Number: 1 Publisher: Nature Publishing Group.
  3. Bourrellier, R. et al. Bright UV Single Photon Emission at Point Defects in h-BN. Nano Letters 16, 4317–4321 (2016). URL https://doi.org/10.1021/acs.nanolett.6b01368. Publisher: American Chemical Society.
  4. Grosso, G. et al. Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride. Nature Communications 8, 705 (2017). URL https://www.nature.com/articles/s41467-017-00810-2. Number: 1 Publisher: Nature Publishing Group.
  5. Fournier, C. et al. Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride. Nature Communications 12, 3779 (2021). URL https://www.nature.com/articles/s41467-021-24019-6. Bandiera_abtest: a Cc_license_type: cc_by Cg_type: Nature Research Journals Number: 1 Primary_atype: Research Publisher: Nature Publishing Group Subject_term: Single photons and quantum effects;Two-dimensional materials Subject_term_id: single-photons-and-quantum-effects;two-dimensional-materials.
  6. Dietrich, A. et al. Observation of fourier transform limited lines in hexagonal boron nitride. Physical Review B 98, 081414 (2018).
  7. Chejanovsky, N. et al. Single-spin resonance in a van der waals embedded paramagnetic defect. Nature materials 20, 1079–1084 (2021).
  8. Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride. Physical Review Letters 119, 057401 (2017). URL https://link.aps.org/doi/10.1103/PhysRevLett.119.057401. Publisher: American Physical Society.
  9. Color Centers in Hexagonal Boron Nitride Monolayers: A Group Theory and Ab Initio Analysis. ACS Photonics 5, 1967–1976 (2018). URL https://doi.org/10.1021/acsphotonics.7b01442. Publisher: American Chemical Society.
  10. Tawfik, S. A. et al. First-principles investigation of quantum emission from hBN defects. Nanoscale 9, 13575–13582 (2017). URL https://pubs.rsc.org/en/content/articlelanding/2017/nr/c7nr04270a. Publisher: The Royal Society of Chemistry.
  11. Mendelson, N. et al. Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride. Nature Materials 20, 321–328 (2021). URL https://www.nature.com/articles/s41563-020-00850-y. Number: 3 Publisher: Nature Publishing Group.
  12. Gottscholl, A. et al. Room temperature coherent control of spin defects in hexagonal boron nitride. Science Advances 7, eabf3630 (2021).
  13. Gottscholl, A. et al. Initialization and read-out of intrinsic spin defects in a van der waals crystal at room temperature. Nature materials 19, 540–545 (2020).
  14. Tran, T. T. et al. Robust multicolor single photon emission from point defects in hexagonal boron nitride. ACS nano 10, 7331–7338 (2016).
  15. Resonant inelastic x-ray scattering studies of elementary excitations. Reviews of Modern Physics 83, 705–767 (2011). URL http://link.aps.org/doi/10.1103/RevModPhys.83.705.
  16. Determining the electron-phonon coupling strength from Resonant Inelastic X-ray Scattering at transition metal L-edges. EPL (Europhysics Letters) 95, 27008 (2011). URL https://iopscience.iop.org/article/10.1209/0295-5075/95/27008.
  17. Dynamics of resonant x-ray and Auger scattering. Reviews of Modern Physics 93, 035001 (2021). URL https://link.aps.org/doi/10.1103/RevModPhys.93.035001.
  18. Towards 10 meV resolution: The design of an ultrahigh resolution soft X-ray RIXS spectrometer. Review of Scientific Instruments 87, 115109 (2016). URL http://aip.scitation.org/doi/10.1063/1.4964847.
  19. Pelliciari, J. et al. Tuning spin excitations in magnetic films by confinement. Nature Materials 20, 188–193 (2021). URL https://www.nature.com/articles/s41563-020-00878-0. Number: 2 Publisher: Nature Publishing Group.
  20. Pelliciari, J. et al. Evolution of spin excitations from bulk to monolayer FeSe. Nature Communications 12, 3122 (2021). URL https://www.nature.com/articles/s41467-021-23317-3. Number: 1 Publisher: Nature Publishing Group.
  21. Dean, M. P. M. et al. Spin excitations in a single La2CuO4 layer. Nature Materials 11, 850–854 (2012). URL http://www.nature.com/nmat/journal/v11/n10/full/nmat3409.html.
  22. Influence of point defects on the near edge structure of hexagonal boron nitride. Physical Review B 96, 144106 (2017). URL https://link.aps.org/doi/10.1103/PhysRevB.96.144106. Publisher: American Physical Society.
  23. Resonant x-ray emission of hexagonal boron nitride. Physical Review B 96, 205116 (2017). URL https://link.aps.org/doi/10.1103/PhysRevB.96.205116.
  24. The Near Edge Structure of Hexagonal Boron Nitride. Microscopy and Microanalysis 20, 1053–1059 (2014). URL https://www.cambridge.org/core/product/identifier/S1431927614000737/type/journal_article.
  25. Direct-bandgap properties and evidence for ultraviolet lasing of hexagonal boron nitride single crystal. Nature materials 3, 404–409 (2004).
  26. Xu, Z.-Q. et al. Single photon emission from plasma treated 2D hexagonal boron nitride. Nanoscale 10, 7957–7965 (2018). URL https://pubs.rsc.org/en/content/articlelanding/2018/nr/c7nr08222c. Publisher: The Royal Society of Chemistry.
  27. Serrano, J. et al. Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and Ab Initio Calculations. Physical Review Letters 98, 095503 (2007). URL https://link.aps.org/doi/10.1103/PhysRevLett.98.095503.
  28. Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling. Physical Review B 98, 214305 (2018). URL https://link.aps.org/doi/10.1103/PhysRevB.98.214305.
  29. Generalization of the Franck-Condon model for phonon excitations by resonant inelastic x-ray scattering. Physical Review B 101, 214307 (2020). URL https://link.aps.org/doi/10.1103/PhysRevB.101.214307.
  30. Feng, X. et al. Disparate Exciton-Phonon Couplings for Zone-Center and Boundary Phonons in Solid-State Graphite. Physical Review Letters 125, 116401 (2020). URL https://link.aps.org/doi/10.1103/PhysRevLett.125.116401. Publisher: American Physical Society.
  31. Dashwood, C. et al. Probing Electron-Phonon Interactions Away from the Fermi Level with Resonant Inelastic X-Ray Scattering. Physical Review X 11, 041052 (2021). URL https://link.aps.org/doi/10.1103/PhysRevX.11.041052.
  32. Kjellsson, L. et al. Resonant inelastic x-ray scattering at the n 2 π𝜋\piitalic_π* resonance: Lifetime-vibrational interference, radiative electron rearrangement, and wave-function imaging. Physical Review A 103, 022812 (2021).
  33. Lindblad, R. et al. X-ray absorption spectrum of the n 2+ molecular ion. Physical Review Letters 124, 203001 (2020).
  34. Resonant inelastic x-ray scattering studies of elementary excitations. Reviews of Modern Physics 83, 705 (2011).
  35. Lee, J. et al. Charge-orbital-lattice coupling effects in the d d excitation profile of one-dimensional cuprates. Physical Review B 89, 041104 (2014).
  36. Martinelli, L. et al. Collective nature of orbital excitations in layered cuprates in the absence of apical oxygens. arXiv preprint arXiv:2304.02115 (2023).
  37. Comtet, J. et al. Wide-field spectral super-resolution mapping of optically active defects in hexagonal boron nitride. Nano letters 19, 2516–2523 (2019).
  38. Hayee, F. et al. Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy. Nature materials 19, 534–539 (2020).
  39. Mendelson, N. et al. Engineering and tuning of quantum emitters in few-layer hexagonal boron nitride. ACS nano 13, 3132–3140 (2019).
  40. Camphausen, R. et al. Observation of near-infrared sub-Poissonian photon emission in hexagonal boron nitride at room temperature. APL Photonics 5, 076103 (2020). URL https://aip.scitation.org/doi/10.1063/5.0008242. Publisher: American Institute of Physics.
  41. Quantum Emitters in Hexagonal Boron Nitride Have Spectrally Tunable Quantum Efficiency. Advanced Materials 30, 1704237 (2018). URL https://onlinelibrary.wiley.com/doi/10.1002/adma.201704237.
  42. Grosso, G. et al. Low-temperature electron–phonon interaction of quantum emitters in hexagonal boron nitride. ACS Photonics 7, 1410–1417 (2020).
  43. Strain-induced modification of the optical characteristics of quantum emitters in hexagonal boron nitride. Advanced Materials 32, 1908316 (2020).
  44. Nikolay, N. et al. Very large and reversible stark-shift tuning of single emitters in layered hexagonal boron nitride. Physical Review Applied 11, 041001 (2019).
  45. Williams, F. Donor—acceptor pairs in semiconductors. physica status solidi (b) 25, 493–512 (1968). URL https://onlinelibrary.wiley.com/doi/abs/10.1002/pssb.19680250202. eprint https://onlinelibrary.wiley.com/doi/pdf/10.1002/pssb.19680250202.
  46. Tan, Q. et al. Donor–Acceptor Pair Quantum Emitters in Hexagonal Boron Nitride. Nano Letters 22, 1331–1337 (2022). URL https://pubs.acs.org/doi/10.1021/acs.nanolett.1c04647.
  47. Dielectric properties of hexagonal boron nitride and transition metal dichalcogenides: from monolayer to bulk. npj 2D Materials and Applications 2, 1–7 (2018).
  48. Native point defects and impurities in hexagonal boron nitride. Physical Review B 97, 214104 (2018).
  49. Hayee, F. et al. Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy. Nature Materials 19, 534–539 (2020). URL https://www.nature.com/articles/s41563-020-0616-9. Number: 5 Publisher: Nature Publishing Group.
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