Elementary excitations of single-photon emitters in hexagonal boron nitride

Pelliciari, Jonathan; Mejia, Enrique; Woods, John M.; Gu, Yanhong; Li, Jiemin; Chand, Saroj B.; Fan, Shiyu; Watanabe, Kenji; Taniguchi, Takashi; Bisogni, Valentina; Grosso, Gabriele

doi:10.1038/s41563-024-01866-4

Elementary excitations of single-photon emitters in hexagonal boron nitride

Journal Article · Tue Apr 23 00:00:00 EDT 2024 · Nature Materials

DOI:https://doi.org/10.1038/s41563-024-01866-4· OSTI ID:2352190

^[1]; Mejia, Enrique ^[2]; Woods, John M. ^[2]; Gu, Yanhong ^[1]; Li, Jiemin ^[1]; ^[2]; ^[1]; ^[3]; ^[3]; ^[1]; ^[2]

Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
City Univ. of New York (CUNY), NY (United States)
National Institute for Materials Science (NIMS), Tsukuba (Japan)

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. Although 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 π* anti-bonding orbitals in shaping the electronic states of the emitters. Importantly, the discovery of elementary excitations in hBN provides fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2352190

Report Number(s):: BNL--225618-2024-JAAM

Journal Information:: Nature Materials, Journal Name: Nature Materials Vol. 23; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Quantum Emitters in Hexagonal Boron Nitride Have Spectrally Tunable Quantum Efficiency Schell, Andreas W.; Svedendahl, Mikael; Quidant, Romain Advanced Materials, Vol. 30, Issue 14 https://doi.org/10.1002/adma.201704237	journal	February 2018
Strain‐Induced Modification of the Optical Characteristics of Quantum Emitters in Hexagonal Boron Nitride Mendelson, Noah; Doherty, Marcus; Toth, Milos Advanced Materials, Vol. 32, Issue 21 https://doi.org/10.1002/adma.201908316	journal	April 2020
Donor—acceptor pairs in semiconductors Williams, F. Physica Status Solidi (b), Vol. 25, Issue 2 https://doi.org/10.1002/pssb.19680250202	journal	January 1968
The Near Edge Structure of Hexagonal Boron Nitride McDougall, Nicholas L.; Nicholls, Rebecca J.; Partridge, Jim G. Microscopy and Microanalysis, Vol. 20, Issue 4 https://doi.org/10.1017/S1431927614000737	journal	April 2014
Donor–Acceptor Pair Quantum Emitters in Hexagonal Boron Nitride Tan, Qinghai; Lai, Jia-Min; Liu, Xue-Lu Nano Letters, Vol. 22, Issue 3 https://doi.org/10.1021/acs.nanolett.1c04647	journal	January 2022
Bright UV Single Photon Emission at Point Defects in h -BN Bourrellier, Romain; Meuret, Sophie; Tararan, Anna Nano Letters, Vol. 16, Issue 7 https://doi.org/10.1021/acs.nanolett.6b01368	journal	June 2016
Wide-Field Spectral Super-Resolution Mapping of Optically Active Defects in Hexagonal Boron Nitride Comtet, Jean; Glushkov, Evgenii; Navikas, Vytautas Nano Letters, Vol. 19, Issue 4 https://doi.org/10.1021/acs.nanolett.9b00178	journal	March 2019
Robust Multicolor Single Photon Emission from Point Defects in Hexagonal Boron Nitride Tran, Toan Trong; Elbadawi, Christopher; Totonjian, Daniel ACS Nano, Vol. 10, Issue 8 https://doi.org/10.1021/acsnano.6b03602	journal	July 2016
Engineering and Tuning of Quantum Emitters in Few-Layer Hexagonal Boron Nitride Mendelson, Noah; Xu, Zai-Quan; Tran, Toan Trong ACS Nano, Vol. 13, Issue 3 https://doi.org/10.1021/acsnano.8b08511	journal	February 2019
Color Centers in Hexagonal Boron Nitride Monolayers: A Group Theory and Ab Initio Analysis Abdi, Mehdi; Chou, Jyh-Pin; Gali, Adam ACS Photonics, Vol. 5, Issue 5 https://doi.org/10.1021/acsphotonics.7b01442	journal	April 2018
Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride Grosso, Gabriele; Moon, Hyowon; Ciccarino, Christopher J. ACS Photonics, Vol. 7, Issue 6 https://doi.org/10.1021/acsphotonics.9b01789	journal	May 2020
Direct-bandgap properties and evidence for ultraviolet lasing of hexagonal boron nitride single crystal Watanabe, Kenji; Taniguchi, Takashi; Kanda, Hisao Nature Materials, Vol. 3, Issue 6 https://doi.org/10.1038/nmat1134	journal	May 2004
Spin excitations in a single La2CuO4 layer Dean, M. P. M.; Springell, R. S.; Monney, C. Nature Materials, Vol. 11, Issue 10 https://doi.org/10.1038/nmat3409	journal	September 2012
Quantum emission from hexagonal boron nitride monolayers Tran, Toan Trong; Bray, Kerem; Ford, Michael J. Nature Nanotechnology, Vol. 11, Issue 1 https://doi.org/10.1038/nnano.2015.242	journal	October 2015
Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride Grosso, Gabriele; Moon, Hyowon; Lienhard, Benjamin Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00810-2	journal	September 2017
Evolution of spin excitations from bulk to monolayer FeSe Pelliciari, Jonathan; Karakuzu, Seher; Song, Qi Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23317-3	journal	May 2021
Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride Fournier, Clarisse; Plaud, Alexandre; Roux, Sébastien Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-24019-6	journal	June 2021
Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride Mendelson, Noah; Chugh, Dipankar; Reimers, Jeffrey R. Nature Materials, Vol. 20, Issue 3 https://doi.org/10.1038/s41563-020-00850-y	journal	November 2020
Tuning spin excitations in magnetic films by confinement Pelliciari, Jonathan; Lee, Sangjae; Gilmore, Keith Nature Materials, Vol. 20, Issue 2 https://doi.org/10.1038/s41563-020-00878-0	journal	January 2021
Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy Hayee, Fariah; Yu, Leo; Zhang, Jingyuan Linda Nature Materials, Vol. 19, Issue 5 https://doi.org/10.1038/s41563-020-0616-9	journal	February 2020
Initialization and read-out of intrinsic spin defects in a van der Waals crystal at room temperature Gottscholl, Andreas; Kianinia, Mehran; Soltamov, Victor Nature Materials, Vol. 19, Issue 5 https://doi.org/10.1038/s41563-020-0619-6	journal	February 2020
Single-spin resonance in a van der Waals embedded paramagnetic defect Chejanovsky, Nathan; Mukherjee, Amlan; Geng, Jianpei Nature Materials, Vol. 20, Issue 8 https://doi.org/10.1038/s41563-021-00979-4	journal	May 2021
Photonics with hexagonal boron nitride Caldwell, Joshua D.; Aharonovich, Igor; Cassabois, Guillaume Nature Reviews Materials, Vol. 4, Issue 8 https://doi.org/10.1038/s41578-019-0124-1	journal	July 2019
Dielectric properties of hexagonal boron nitride and transition metal dichalcogenides: from monolayer to bulk Laturia, Akash; Van de Put, Maarten L.; Vandenberghe, William G. npj 2D Materials and Applications, Vol. 2, Issue 1 https://doi.org/10.1038/s41699-018-0050-x	journal	March 2018
First-principles investigation of quantum emission from hBN defects Tawfik, Sherif Abdulkader; Ali, Sajid; Fronzi, Marco Nanoscale, Vol. 9, Issue 36 https://doi.org/10.1039/C7NR04270A	journal	January 2017
Single photon emission from plasma treated 2D hexagonal boron nitride Xu, Zai-Quan; Elbadawi, Christopher; Tran, Toan Trong Nanoscale, Vol. 10, Issue 17 https://doi.org/10.1039/C7NR08222C	journal	January 2018
Towards 10 meV resolution: The design of an ultrahigh resolution soft X-ray RIXS spectrometer Dvorak, Joseph; Jarrige, Ignace; Bisogni, Valentina Review of Scientific Instruments, Vol. 87, Issue 11 https://doi.org/10.1063/1.4964847	journal	November 2016
Observation of near-infrared sub-Poissonian photon emission in hexagonal boron nitride at room temperature Camphausen, Robin; Marini, Loris; Tawfik, Sherif Abdulkader APL Photonics, Vol. 5, Issue 7 https://doi.org/10.1063/5.0008242	journal	July 2020
Resonant inelastic x-ray scattering at the N 2 π * resonance: Lifetime-vibrational interference, radiative electron rearrangement, and wave-function imaging Kjellsson, L.; Ekholm, V.; Agåker, M. Physical Review A, Vol. 103, Issue 2 https://doi.org/10.1103/PhysRevA.103.022812	journal	February 2021
Very Large and Reversible Stark-Shift Tuning of Single Emitters in Layered Hexagonal Boron Nitride Nikolay, Niko; Mendelson, Noah; Sadzak, Nikola Physical Review Applied, Vol. 11, Issue 4 https://doi.org/10.1103/PhysRevApplied.11.041001	journal	April 2019
Generalization of the Franck-Condon model for phonon excitations by resonant inelastic x-ray scattering Geondzhian, Andrey; Gilmore, Keith Physical Review B, Vol. 101, Issue 21 https://doi.org/10.1103/PhysRevB.101.214307	journal	June 2020
Charge-orbital-lattice coupling effects in the d d excitation profile of one-dimensional cuprates Lee, J. J.; Moritz, B.; Lee, W. S. Physical Review B, Vol. 89, Issue 4 https://doi.org/10.1103/PhysRevB.89.041104	journal	January 2014
Influence of point defects on the near edge structure of hexagonal boron nitride McDougall, Nicholas L.; Partridge, Jim G.; Nicholls, Rebecca J. Physical Review B, Vol. 96, Issue 14 https://doi.org/10.1103/PhysRevB.96.144106	journal	October 2017
Resonant x-ray emission of hexagonal boron nitride Vinson, John; Jach, Terrence; Müller, Matthias Physical Review B, Vol. 96, Issue 20 https://doi.org/10.1103/PhysRevB.96.205116	journal	November 2017
Native point defects and impurities in hexagonal boron nitride Weston, L.; Wickramaratne, D.; Mackoit, M. Physical Review B, Vol. 97, Issue 21 https://doi.org/10.1103/PhysRevB.97.214104	journal	June 2018
Observation of Fourier transform limited lines in hexagonal boron nitride Dietrich, A.; Bürk, M.; Steiger, E. S. Physical Review B, Vol. 98, Issue 8 https://doi.org/10.1103/PhysRevB.98.081414	journal	August 2018
Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling Geondzhian, Andrey; Gilmore, Keith Physical Review B, Vol. 98, Issue 21 https://doi.org/10.1103/PhysRevB.98.214305	journal	December 2018
Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride Jungwirth, Nicholas R.; Fuchs, Gregory D. Physical Review Letters, Vol. 119, Issue 5 https://doi.org/10.1103/PhysRevLett.119.057401	journal	July 2017
X-Ray Absorption Spectrum of the N 2 + Molecular Ion Lindblad, R.; Kjellsson, L.; Couto, R. C. Physical Review Letters, Vol. 124, Issue 20 https://doi.org/10.1103/PhysRevLett.124.203001	journal	May 2020
Disparate Exciton-Phonon Couplings for Zone-Center and Boundary Phonons in Solid-State Graphite Feng, Xuefei; Sallis, Shawn; Shao, Yu-Cheng Physical Review Letters, Vol. 125, Issue 11 https://doi.org/10.1103/PhysRevLett.125.116401	journal	September 2020
Collective Nature of Orbital Excitations in Layered Cuprates in the Absence of Apical Oxygens Martinelli, Leonardo; Wohlfeld, Krzysztof; Pelliciari, Jonathan Physical Review Letters, Vol. 132, Issue 6 https://doi.org/10.1103/PhysRevLett.132.066004	journal	February 2024
Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and Ab Initio Calculations Serrano, J.; Bosak, A.; Arenal, R. Physical Review Letters, Vol. 98, Issue 9 https://doi.org/10.1103/PhysRevLett.98.095503	journal	March 2007
Resonant inelastic x-ray scattering studies of elementary excitations Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P. Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.705	journal	June 2011
Dynamics of resonant x-ray and Auger scattering Gel’mukhanov, Faris; Odelius, Michael; Polyutov, Sergey P. Reviews of Modern Physics, Vol. 93, Issue 3 https://doi.org/10.1103/RevModPhys.93.035001	journal	July 2021
Room temperature coherent control of spin defects in hexagonal boron nitride Gottscholl, Andreas; Diez, Matthias; Soltamov, Victor Science Advances, Vol. 7, Issue 14 https://doi.org/10.1126/sciadv.abf3630	journal	April 2021
Determining the electron-phonon coupling strength from Resonant Inelastic X-ray Scattering at transition metal L-edges Ament, L. J. P.; van Veenendaal, M.; van den Brink, J. EPL (Europhysics Letters), Vol. 95, Issue 2 https://doi.org/10.1209/0295-5075/95/27008	journal	July 2011

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Elementary excitations of single-photon emitters in hexagonal boron nitride

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