Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride
Abstract
Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.
- Authors:
-
[2]
- University of California, Santa Cruz, CA (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- University of California, Santa Cruz, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC); National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1888623
- Report Number(s):
- LLNL-JRNL-820110
Journal ID: ISSN 2057-3960; 1031303; TRN: US2309909
- Grant/Contract Number:
- AC52-07NA27344; DMR-1760260; DMR-1956015; DMR-1747426; SC0012704; AST 1828315; AC02-05CH11231; ACI-1548562
- Resource Type:
- Accepted Manuscript
- Journal Name:
- npj Computational Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2057-3960
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; computational methods; electronic structure; electronics; photonics; device physics; spintronics
Citation Formats
Smart, Tyler J., Li, Kejun, Xu, Junqing, and Ping, Yuan. Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride. United States: N. p., 2021.
Web. doi:10.1038/s41524-021-00525-5.
Smart, Tyler J., Li, Kejun, Xu, Junqing, & Ping, Yuan. Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride. United States. https://doi.org/10.1038/s41524-021-00525-5
Smart, Tyler J., Li, Kejun, Xu, Junqing, and Ping, Yuan. Fri .
"Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride". United States. https://doi.org/10.1038/s41524-021-00525-5. https://www.osti.gov/servlets/purl/1888623.
@article{osti_1888623,
title = {Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride},
author = {Smart, Tyler J. and Li, Kejun and Xu, Junqing and Ping, Yuan},
abstractNote = {Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.},
doi = {10.1038/s41524-021-00525-5},
journal = {npj Computational Materials},
number = 1,
volume = 7,
place = {United States},
year = {Fri Apr 30 00:00:00 EDT 2021},
month = {Fri Apr 30 00:00:00 EDT 2021}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Two-Level Quantum Systems in Two-Dimensional Materials for Single Photon Emission
journal, December 2018
- Gupta, Sunny; Yang, Ji-Hui; Yakobson, Boris I.
- Nano Letters, Vol. 19, Issue 1
Generation of Spin Defects in Hexagonal Boron Nitride
journal, July 2020
- Kianinia, Mehran; White, Simon; Fröch, Johannes E.
- ACS Photonics, Vol. 7, Issue 8
Optical properties of tungsten trioxide from first-principles calculations
journal, April 2013
- Ping, Yuan; Rocca, Dario; Galli, Giulia
- Physical Review B, Vol. 87, Issue 16
Strain‐Induced Modification of the Optical Characteristics of Quantum Emitters in Hexagonal Boron Nitride
journal, April 2020
- Mendelson, Noah; Doherty, Marcus; Toth, Milos
- Advanced Materials, Vol. 32, Issue 21
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
VNCB defect as source of single photon emission from hexagonal boron nitride
journal, June 2020
- Sajid, A.; Thygesen, Kristian S.
- 2D Materials, Vol. 7, Issue 3
The ORCA program system: The ORCA program system
journal, June 2011
- Neese, Frank
- Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 1
Ultrafast optical control of orbital and spin dynamics in a solid-state defect
journal, August 2014
- Bassett, L. C.; Heremans, F. J.; Christle, D. J.
- Science, Vol. 345, Issue 6202
Phonon-induced multicolor correlations in hBN single-photon emitters
journal, January 2019
- Feldman, Matthew A.; Puretzky, Alex; Lindsay, Lucas
- Physical Review B, Vol. 99, Issue 2
First principles calculation of spin-related quantities for point defect qubit research
journal, December 2018
- Ivády, Viktor; Abrikosov, Igor A.; Gali, Adam
- npj Computational Materials, Vol. 4, Issue 1
First principles method for the calculation of zero-field splitting tensors in periodic systems
journal, January 2008
- Rayson, M. J.; Briddon, P. R.
- Physical Review B, Vol. 77, Issue 3
Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides
journal, October 2018
- Refaely-Abramson, Sivan; Qiu, Diana Y.; Louie, Steven G.
- Physical Review Letters, Vol. 121, Issue 16
Structural absorption by barbule microstructures of super black bird of paradise feathers
journal, January 2018
- McCoy, Dakota E.; Feo, Teresa; Harvey, Todd Alan
- Nature Communications, Vol. 9, Issue 1
Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013
- Hamann, D. R.
- Physical Review B, Vol. 88, Issue 8
Quantum emitters in two dimensions
journal, October 2017
- Aharonovich, Igor; Toth, Milos
- Science, Vol. 358, Issue 6360
Solution of the Bethe-Salpeter equation without empty electronic states: Application to the absorption spectra of bulk systems
journal, January 2012
- Rocca, Dario; Ping, Yuan; Gebauer, Ralph
- Physical Review B, Vol. 85, Issue 4
XSEDE: Accelerating Scientific Discovery
journal, September 2014
- Towns, John; Cockerill, Timothy; Dahan, Maytal
- Computing in Science & Engineering, Vol. 16, Issue 5
Exciton radiative lifetime controlled by the lateral confinement energy in a single quantum dot
journal, April 2005
- Hours, J.; Senellart, P.; Peter, E.
- Physical Review B, Vol. 71, Issue 16
First-principles electrostatic potentials for reliable alignment at interfaces and defects
journal, March 2017
- Sundararaman, Ravishankar; Ping, Yuan
- The Journal of Chemical Physics, Vol. 146, Issue 10
JDFTx: Software for joint density-functional theory
journal, January 2017
- Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Schwarz, Kathleen A.
- SoftwareX, Vol. 6
Nonempirical hybrid functionals for band gaps and polaronic distortions in solids
journal, March 2018
- Miceli, Giacomo; Chen, Wei; Reshetnyak, Igor
- Physical Review B, Vol. 97, Issue 12
Quasiparticle band structure based on a generalized Kohn-Sham scheme
journal, September 2007
- Fuchs, F.; Furthmüller, J.; Bechstedt, F.
- Physical Review B, Vol. 76, Issue 11
2D materials for quantum information science
journal, August 2019
- Liu, Xiaolong; Hersam, Mark C.
- Nature Reviews Materials, Vol. 4, Issue 10
Calculation of the zero-field splitting tensor on the basis of hybrid density functional and Hartree-Fock theory
journal, October 2007
- Neese, Frank
- The Journal of Chemical Physics, Vol. 127, Issue 16
Phonon-Induced Population Dynamics and Intersystem Crossing in Nitrogen-Vacancy Centers
journal, April 2015
- Goldman, M. L.; Sipahigil, A.; Doherty, M. W.
- Physical Review Letters, Vol. 114, Issue 14
Electronic Structure and Magnetic Properties of a Titanium(II) Coordination Complex
journal, April 2020
- Zolnhofer, Eva M.; Wijeratne, Gayan B.; Jackson, Timothy A.
- Inorganic Chemistry, Vol. 59, Issue 9
Predicting Phosphorescence Rates of Light Organic Molecules Using Time-Dependent Density Functional Theory and the Path Integral Approach to Dynamics
journal, February 2019
- de Souza, Bernardo; Farias, Giliandro; Neese, Frank
- Journal of Chemical Theory and Computation, Vol. 15, Issue 3
First-principles calculations for defects and impurities: Applications to III-nitrides
journal, April 2004
- Van de Walle, Chris G.; Neugebauer, Jörg
- Journal of Applied Physics, Vol. 95, Issue 8
Polarization and Localization of Single-Photon Emitters in Hexagonal Boron Nitride Wrinkles
journal, July 2020
- Yim, Donggyu; Yu, Mihyang; Noh, Gichang
- ACS Applied Materials & Interfaces, Vol. 12, Issue 32
Dimensionality and anisotropicity dependence of radiative recombination in nanostructured phosphorene
journal, January 2019
- Wu, Feng; Rocca, Dario; Ping, Yuan
- Journal of Materials Chemistry C, Vol. 7, Issue 41
Determination of Formation and Ionization Energies of Charged Defects in Two-Dimensional Materials
journal, May 2015
- Wang, Dan; Han, Dong; Li, Xian-Bin
- Physical Review Letters, Vol. 114, Issue 19
Quantum computing with defects
journal, April 2010
- Weber, J. R.; Koehl, W. F.; Varley, J. B.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 19
Spinning up quantum defects in 2D materials
journal, April 2020
- Turiansky, M. E.; Alkauskas, A.; Van de Walle, C. G.
- Nature Materials, Vol. 19, Issue 5
Wannier Koopmans Method Calculations of 2D Material Band Gaps
journal, January 2018
- Weng, Mouyi; Li, Sibai; Zheng, Jiaxin
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 2
Ab initio calculations of absorption spectra of semiconducting nanowires within many-body perturbation theory
journal, January 2012
- Ping, Yuan; Rocca, Dario; Lu, Deyu
- Physical Review B, Vol. 85, Issue 3
Substitutional Si impurities in monolayer hexagonal boron nitride
journal, August 2019
- Ahmadpour Monazam, Mohammad Reza; Ludacka, Ursula; Komsa, Hannu-Pekka
- Applied Physics Letters, Vol. 115, Issue 7
Dangling Bonds in Hexagonal Boron Nitride as Single-Photon Emitters
journal, September 2019
- Turiansky, Mark E.; Alkauskas, Audrius; Bassett, Lee C.
- Physical Review Letters, Vol. 123, Issue 12
Layer dependence of defect charge transition levels in two-dimensional materials
journal, February 2020
- Wang, Dan; Sundararaman, Ravishankar
- Physical Review B, Vol. 101, Issue 5
Carbon dimer defect as a source of the 4.1 eV luminescence in hexagonal boron nitride
journal, November 2019
- Mackoit-Sinkevičienė, M.; Maciaszek, M.; Van de Walle, C. G.
- Applied Physics Letters, Vol. 115, Issue 21
Nonmagnetic Quantum Emitters in Boron Nitride with Ultranarrow and Sideband-Free Emission Spectra
journal, May 2017
- Li, Xiangzhi; Shepard, Gabriella D.; Cupo, Andrew
- ACS Nano, Vol. 11, Issue 7
Coupling Quantum Emitters in 2D Materials with Tapered Fibers
journal, March 2017
- Schell, Andreas W.; Takashima, Hideaki; Tran, Toan Trong
- ACS Photonics, Vol. 4, Issue 4
Properties of nitrogen-vacancy centers in diamond: the group theoretic approach
journal, February 2011
- Maze, J. R.; Gali, A.; Togan, E.
- New Journal of Physics, Vol. 13, Issue 2
Room temperature coherent control of defect spin qubits in silicon carbide
journal, November 2011
- Koehl, William F.; Buckley, Bob B.; Heremans, F. Joseph
- Nature, Vol. 479, Issue 7371
Fundamental principles for calculating charged defect ionization energies in ultrathin two-dimensional materials
journal, December 2018
- Smart, Tyler J.; Wu, Feng; Govoni, Marco
- Physical Review Materials, Vol. 2, Issue 12
Carrier recombination mechanism at defects in wide band gap two-dimensional materials from first principles
journal, August 2019
- Wu, Feng; Smart, Tyler J.; Xu, Junqing
- Physical Review B, Vol. 100, Issue 8
Designing defect-based qubit candidates in wide-gap binary semiconductors for solid-state quantum technologies
journal, December 2017
- Seo, Hosung; Ma, He; Govoni, Marco
- Physical Review Materials, Vol. 1, Issue 7
First-principles engineering of charged defects for two-dimensional quantum technologies
journal, December 2017
- Wu, Feng; Galatas, Andrew; Sundararaman, Ravishankar
- Physical Review Materials, Vol. 1, Issue 7
Electronic excitations in light absorbers for photoelectrochemical energy conversion: first principles calculations based on many body perturbation theory
journal, January 2013
- Ping, Yuan; Rocca, Dario; Galli, Giulia
- Chemical Society Reviews, Vol. 42, Issue 6
Ab initio calculation of spin-orbit coupling for an NV center in diamond exhibiting dynamic Jahn-Teller effect
journal, August 2017
- Thiering, Gergő; Gali, Adam
- Physical Review B, Vol. 96, Issue 8
Optically Addressing Single Rare-Earth Ions in a Nanophotonic Cavity
journal, October 2018
- Zhong, Tian; Kindem, Jonathan M.; Bartholomew, John G.
- Physical Review Letters, Vol. 121, Issue 18
Large Scale GW Calculations
journal, May 2015
- Govoni, Marco; Galli, Giulia
- Journal of Chemical Theory and Computation, Vol. 11, Issue 6
Initialization and read-out of intrinsic spin defects in a van der Waals crystal at room temperature
journal, February 2020
- Gottscholl, Andreas; Kianinia, Mehran; Soltamov, Victor
- Nature Materials, Vol. 19, Issue 5
yambo: An ab initio tool for excited state calculations
journal, August 2009
- Marini, Andrea; Hogan, Conor; Grüning, Myrta
- Computer Physics Communications, Vol. 180, Issue 8
Spin coherence in two-dimensional materials
journal, April 2019
- Ye, Meng; Seo, Hosung; Galli, Giulia
- npj Computational Materials, Vol. 5, Issue 1
U1 snRNP regulates cancer cell migration and invasion in vitro
journal, January 2020
- Oh, Jung-Min; Venters, Christopher C.; Di, Chao
- Nature Communications, Vol. 11, Issue 1