skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy

Abstract

Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure challenge their technological utility. Here, we directly correlate hBN quantum emission with local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nanobeam electron diffraction. Across 40 emitters, we observe zero phonon lines (ZPLs) in PL and CL ranging from 540 to 720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, at least four distinct defect classes are responsible for the observed emission range, and all four classes are stable upon both optical and electron illumination. Our findings offer a foundation for future atomic-scale optical characterization of colour centres.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3];  [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [1]
  1. Stanford Univ., CA (United States)
  2. Harvard Univ., Cambridge, MA (United States)
  3. Univ. of Technology Sydney, NSW (Australia)
  4. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits (PTL); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; Betty and Gordon Moore Foundation (BGMF)
OSTI Identifier:
1608703
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 19; Journal Issue: 5; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Hayee, Fariah, Yu, Leo, Zhang, Jingyuan Linda, Ciccarino, Christopher J., Nguyen, Minh, Marshall, Ann F., Aharonovich, Igor, Vučković, Jelena, Narang, Prineha, Heinz, Tony F., and Dionne, Jennifer A. Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy. United States: N. p., 2020. Web. doi:10.1038/s41563-020-0616-9.
Hayee, Fariah, Yu, Leo, Zhang, Jingyuan Linda, Ciccarino, Christopher J., Nguyen, Minh, Marshall, Ann F., Aharonovich, Igor, Vučković, Jelena, Narang, Prineha, Heinz, Tony F., & Dionne, Jennifer A. Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy. United States. doi:https://doi.org/10.1038/s41563-020-0616-9
Hayee, Fariah, Yu, Leo, Zhang, Jingyuan Linda, Ciccarino, Christopher J., Nguyen, Minh, Marshall, Ann F., Aharonovich, Igor, Vučković, Jelena, Narang, Prineha, Heinz, Tony F., and Dionne, Jennifer A. Mon . "Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy". United States. doi:https://doi.org/10.1038/s41563-020-0616-9. https://www.osti.gov/servlets/purl/1608703.
@article{osti_1608703,
title = {Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy},
author = {Hayee, Fariah and Yu, Leo and Zhang, Jingyuan Linda and Ciccarino, Christopher J. and Nguyen, Minh and Marshall, Ann F. and Aharonovich, Igor and Vučković, Jelena and Narang, Prineha and Heinz, Tony F. and Dionne, Jennifer A.},
abstractNote = {Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, but their large spectral variability and unknown local structure challenge their technological utility. Here, we directly correlate hBN quantum emission with local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nanobeam electron diffraction. Across 40 emitters, we observe zero phonon lines (ZPLs) in PL and CL ranging from 540 to 720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, at least four distinct defect classes are responsible for the observed emission range, and all four classes are stable upon both optical and electron illumination. Our findings offer a foundation for future atomic-scale optical characterization of colour centres.},
doi = {10.1038/s41563-020-0616-9},
journal = {Nature Materials},
number = 5,
volume = 19,
place = {United States},
year = {2020},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy
journal, September 2017


Tunable and high-purity room temperature single-photon emission from atomic defects in hexagonal boron nitride
journal, September 2017


Point defects in hexagonal boron nitride. I. EPR, thermoluminescence, and thermally-stimulated-current measurements
journal, March 1975


Material platforms for spin-based photonic quantum technologies
journal, April 2018


Efficient single photon emission from a high-purity hexagonal boron nitride crystal
journal, September 2016


Robust Multicolor Single Photon Emission from Point Defects in Hexagonal Boron Nitride
journal, July 2016

  • Tran, Toan Trong; Elbadawi, Christopher; Totonjian, Daniel
  • ACS Nano, Vol. 10, Issue 8
  • DOI: 10.1021/acsnano.6b03602

Optical Signatures of Quantum Emitters in Suspended Hexagonal Boron Nitride
journal, February 2017

  • Exarhos, Annemarie L.; Hopper, David A.; Grote, Richard R.
  • ACS Nano, Vol. 11, Issue 3
  • DOI: 10.1021/acsnano.7b00665

Single photon emitters in boron nitride: More than a supplementary material
journal, March 2018


Quantum emission from hexagonal boron nitride monolayers
journal, October 2015

  • Tran, Toan Trong; Bray, Kerem; Ford, Michael J.
  • Nature Nanotechnology, Vol. 11, Issue 1
  • DOI: 10.1038/nnano.2015.242

Imaging of Optically Active Defects with Nanometer Resolution
journal, February 2018


Bright UV Single Photon Emission at Point Defects in h -BN
journal, June 2016


Temperature Dependence of Wavelength Selectable Zero-Phonon Emission from Single Defects in Hexagonal Boron Nitride
journal, September 2016


High-sensitivity diamond magnetometer with nanoscale resolution
journal, September 2008

  • Taylor, J. M.; Cappellaro, P.; Childress, L.
  • Nature Physics, Vol. 4, Issue 10
  • DOI: 10.1038/nphys1075

Structural Attributes and Photodynamics of Visible Spectrum Quantum Emitters in Hexagonal Boron Nitride
journal, October 2016


Atomic localization of quantum emitters in multilayer hexagonal boron nitride
journal, January 2019

  • Vogl, Tobias; Doherty, Marcus W.; Buchler, Ben C.
  • Nanoscale, Vol. 11, Issue 30
  • DOI: 10.1039/C9NR04269E

Quantum technologies with optically interfaced solid-state spins
journal, August 2018


Photon Bunching in Cathodoluminescence
journal, May 2015


Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride
journal, July 2017


Atomically thin hexagonal boron nitride probed by ultrahigh-resolution transmission electron microscopy
journal, October 2009


Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides
journal, July 2019


Engineering and Localization of Quantum Emitters in Large Hexagonal Boron Nitride Layers
journal, October 2016

  • Choi, Sumin; Tran, Toan Trong; Elbadawi, Christopher
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 43
  • DOI: 10.1021/acsami.6b09875

Understanding and Calibrating Density-Functional-Theory Calculations Describing the Energy and Spectroscopy of Defect Sites in Hexagonal Boron Nitride
journal, February 2018

  • Reimers, Jeffrey R.; Sajid, A.; Kobayashi, Rika
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 3
  • DOI: 10.1021/acs.jctc.7b01072

Anomalous Pressure Characteristics of Defects in Hexagonal Boron Nitride Flakes
journal, June 2018


Quantum Emitters in Hexagonal Boron Nitride Have Spectrally Tunable Quantum Efficiency
journal, February 2018

  • Schell, Andreas W.; Svedendahl, Mikael; Quidant, Romain
  • Advanced Materials, Vol. 30, Issue 14
  • DOI: 10.1002/adma.201704237

Characterization and manipulation of individual defects in insulating hexagonal boron nitride using scanning tunnelling microscopy
journal, August 2015


Nanometre-scale thermometry in a living cell
journal, July 2013


Fabrication of a Freestanding Boron Nitride Single Layer and Its Defect Assignments
journal, May 2009


Native point defects and impurities in hexagonal boron nitride
journal, June 2018


Nanoscale nuclear magnetic resonance with chemical resolution
journal, June 2017


Selective Sputtering and Atomic Resolution Imaging of Atomically Thin Boron Nitride Membranes
journal, July 2009

  • Meyer, Jannik C.; Chuvilin, Andrey; Algara-Siller, Gerardo
  • Nano Letters, Vol. 9, Issue 7
  • DOI: 10.1021/nl9011497

Quantum internet: A vision for the road ahead
journal, October 2018


First-principles investigation of quantum emission from hBN defects
journal, January 2017

  • Tawfik, Sherif Abdulkader; Ali, Sajid; Fronzi, Marco
  • Nanoscale, Vol. 9, Issue 36
  • DOI: 10.1039/C7NR04270A

Satellite-to-ground quantum key distribution
journal, August 2017

  • Liao, Sheng-Kai; Cai, Wen-Qi; Liu, Wei-Yue
  • Nature, Vol. 549, Issue 7670
  • DOI: 10.1038/nature23655

Hexagonal boron nitride is an indirect bandgap semiconductor
journal, January 2016


Triangle defect states of hexagonal boron nitride atomic layer: Density functional theory calculations
journal, April 2010


Electron knock-on damage in hexagonal boron nitride monolayers
journal, September 2010