Discovery of atomic clock-like spin defects in simple oxides from first principles.
Journal
Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555
Informations de publication
Date de publication:
06 Jun 2024
06 Jun 2024
Historique:
received:
15
02
2023
accepted:
17
05
2024
medline:
7
6
2024
pubmed:
7
6
2024
entrez:
6
6
2024
Statut:
epublish
Résumé
Virtually noiseless due to the scarcity of spinful nuclei in the lattice, simple oxides hold promise as hosts of solid-state spin qubits. However, no suitable spin defect has yet been found in these systems. Using high-throughput first-principles calculations, we predict spin defects in calcium oxide with electronic properties remarkably similar to those of the NV center in diamond. These defects are charged complexes where a dopant atom - Sb, Bi, or I - occupies the volume vacated by adjacent cation and anion vacancies. The predicted zero phonon line shows that the Bi complex emits in the telecommunication range, and the computed many-body energy levels suggest a viable optical cycle required for qubit initialization. Notably, the high-spin nucleus of each dopant strongly couples to the electron spin, leading to many controllable quantum levels and the emergence of atomic clock-like transitions that are well protected from environmental noise. Specifically, the Hanh-echo coherence time increases beyond seconds at the clock-like transition in the defect with
Identifiants
pubmed: 38844443
doi: 10.1038/s41467-024-49057-8
pii: 10.1038/s41467-024-49057-8
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
4812Subventions
Organisme : Vetenskapsrådet (Swedish Research Council)
ID : 2022-00276
Organisme : Knut och Alice Wallenbergs Stiftelse (Knut and Alice Wallenberg Foundation)
ID : 2018.0071
Informations de copyright
© 2024. The Author(s).
Références
Zhang, G., Cheng, Y., Chou, J.-P. & Gali, A. Material platforms for defect qubits and single-photon emitters. Appl. Phys. Rev. 7, 031308 (2020).
doi: 10.1063/5.0006075
Wolfowicz, G. et al. Quantum guidelines for solid-state spin defects. Nat. Rev. Mater. 6, 906–925 (2021).
doi: 10.1038/s41578-021-00306-y
Davies, G., Hamer, M. F. & Price, W. C. Optical studies of the 1.945 eV vibronic band in diamond. Proc. R. Soc. Lond. A. Math. Phys. Sci. 348, 285–298 (1976).
Balasubramanian, G. et al. Ultralong spin coherence time in isotopically engineered diamond. Nat. Mater. 8, 383–387 (2009).
pubmed: 19349970
doi: 10.1038/nmat2420
Choi, S., Jain, M. & Louie, S. G. Mechanism for optical initialization of spin in NV
doi: 10.1103/PhysRevB.86.041202
Doherty, M. W., Manson, N. B., Delaney, P. & Hollenberg, L. C. L. The negatively charged nitrogen-vacancy centre in diamond: The electronic solution. N. J. Phys. 13, 025019 (2011).
doi: 10.1088/1367-2630/13/2/025019
Goldman, M. L. et al. State-selective intersystem crossing in nitrogen-vacancy centers. Phys. Rev. B 91, 165201 (2015).
doi: 10.1103/PhysRevB.91.165201
Maze, J. R. et al. Properties of nitrogen-vacancy centers in diamond: The group theoretic approach. N. J. Phys. 13, 025025 (2011).
doi: 10.1088/1367-2630/13/2/025025
Rogers, L. J., Armstrong, S., Sellars, M. J. & Manson, N. B. Infrared emission of the NV centre in diamond: Zeeman and uniaxial stress studies. N. J. Phys. 10, 103024 (2008).
doi: 10.1088/1367-2630/10/10/103024
Ma, H., Sheng, N., Govoni, M. & Galli, G. First-principles studies of strongly correlated states in defect spin qubits in diamond. Phys. Chem. Chem. Phys. 22, 25522–25527 (2020).
pubmed: 33084673
doi: 10.1039/D0CP04585C
Davidsson, J. et al. First principles predictions of magneto-optical data for semiconductor point defect identification: the case of divacancy defects in 4h-sic. N. J. Phys. 20, 023035 (2018).
doi: 10.1088/1367-2630/aaa752
Davidsson, J. et al. Identification of divacancy and silicon vacancy qubits in 6h-sic. Appl. Phys. Lett. 114, 112107 (2019).
doi: 10.1063/1.5083031
Seo, H. et al. Quantum decoherence dynamics of divacancy spins in silicon carbide. Nat. Commun. 7, 12935 (2016).
pubmed: 27679936
pmcid: 5056425
doi: 10.1038/ncomms12935
Christle, D. J. et al. Isolated electron spins in silicon carbide with millisecond coherence times. Nat. Mater. 14, 160–163 (2015).
pubmed: 25437259
doi: 10.1038/nmat4144
Kanai, S. et al. Generalized scaling of spin qubit coherence in over 12,000 host materials. Proc. Natl Acad. Sci. 119, e2121808119 (2022).
pubmed: 35385350
pmcid: 9169712
doi: 10.1073/pnas.2121808119
Ferrenti, A. M., de Leon, N. P., Thompson, J. D. & Cava, R. J. Identifying candidate hosts for quantum defects via data mining. npj Comput. Mater. 6, 126 (2020).
doi: 10.1038/s41524-020-00391-7
Davidsson, J., Ivády, V., Armiento, R. & Abrikosov, I. A. Adaq: Automatic workflows for magneto-optical properties of point defects in semiconductors. Comput. Phys. Commun. 269, 108091 (2021).
doi: 10.1016/j.cpc.2021.108091
Adaq. https://httk.org/adaq/ (2022). Accessed: 2022-04-04.
Sheng, N., Vorwerk, C., Govoni, M. & Galli, G. Green’s Function Formulation of Quantum Defect Embedding Theory. J. Chem. Theory Comput. 18, 3512–3522 (2022).
pubmed: 35648660
doi: 10.1021/acs.jctc.2c00240
Ma, H., Sheng, N., Govoni, M. & Galli, G. Quantum Embedding Theory for Strongly Correlated States in Materials. J. Chem. Theory Comput. 17, 2116–2125 (2021).
pubmed: 33739106
doi: 10.1021/acs.jctc.0c01258
Onizhuk, M. & Galli, G. Pycce: A python package for cluster correlation expansion simulations of spin qubit dynamics. Adv. Theory Simul. 4, 2100254 (2021).
doi: 10.1002/adts.202100254
Davidsson, J. Color Centers in Semiconductors for Quantum Applications: A High-Throughput Search of Point Defects in SiC. Ph.D. thesis (Linköping University Electronic Press, 2021). http://urn.kb.se/resolve?urn=urn%3Anbn%3Ase%3Aliu%3Adiva-173108 .
Davidsson, J. et al. Exhaustive characterization of modified si vacancies in 4h-sic. Nanophotonics 11, 4565–4580 (2022).
doi: 10.1515/nanoph-2022-0400
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
pubmed: 10062328
doi: 10.1103/PhysRevLett.77.3865
Stavale, F. et al. Donor characteristics of transition-metal-doped oxides: Cr-doped mgo versus mo-doped cao. J. Am. Chem. Soc. 134, 11380–11383 (2012).
pubmed: 22741775
doi: 10.1021/ja304497n
Lang, D. V. Deep-level transient spectroscopy: A new method to characterize traps in semiconductors. J. Appl. Phys. 45, 3023–3032 (2003).
doi: 10.1063/1.1663719
Gali, Á. Ab initio theory of the nitrogen-vacancy center in diamond. Nanophotonics 8, 1907–1943 (2019).
doi: 10.1515/nanoph-2019-0154
Whited, R., Flaten, C. J. & Walker, W. Exciton thermoreflectance of mgo and cao. Solid State Commun. 13, 1903–1905 (1973).
doi: 10.1016/0038-1098(73)90754-0
Wolfowicz, G. et al. Atomic clock transitions in silicon-based spin qubits. Nat. Nanotechnol. 8, 561–564 (2013).
pubmed: 23793304
doi: 10.1038/nnano.2013.117
Onizhuk, M. et al. Probing the coherence of solid-state qubits at avoided crossings. PRX Quantum 2, 010311 (2021).
doi: 10.1103/PRXQuantum.2.010311
Balian, S. J., Wolfowicz, G., Morton, J. J. L. & Monteiro, T. S. Quantum-bath-driven decoherence of mixed spin systems. Phys. Rev. B 89, 045403 (2014).
doi: 10.1103/PhysRevB.89.045403
Davies, G. & Hamer, M. Optical studies of the 1.945 ev vibronic band in diamond. Proc. R. Soc. Lond. A. Math. Phys. Sci. 348, 285–298 (1976).
Ulbricht, R. & Loh, Z.-H. Excited-state lifetime of the Nv
doi: 10.1103/PhysRevB.98.094309
Batalov, A. et al. Temporal coherence of photons emitted by single nitrogen-vacancy defect centers in diamond using optical rabi-oscillations. Phys. Rev. Lett. 100, 077401 (2008).
pubmed: 18352594
doi: 10.1103/PhysRevLett.100.077401
Gasca, L. From o to l: The future of optical-wavelength bands. Broadband Prop. 6, 83–85 (2008).
Alkauskas, A., Buckley, B. B., Awschalom, D. D. & de Walle, C. G. V. First-principles theory of the luminescence lineshape for the triplet transition in diamond nv centres. N. J. Phys. 16, 073026 (2014).
doi: 10.1088/1367-2630/16/7/073026
Lee, J. H. et al. Strong zero-phonon transition from point defect-stacking fault complexes in silicon carbide nanowires. Nano Lett. 21, 9187–9194 (2021).
pubmed: 34677068
doi: 10.1021/acs.nanolett.1c03013
Ivády, V., Simon, T., Maze, J. R., Abrikosov, I. A. & Gali, A. Pressure and temperature dependence of the zero-field splitting in the ground state of nv centers in diamond: A first-principles study. Phys. Rev. B 90, 235205 (2014).
doi: 10.1103/PhysRevB.90.235205
Losego, M. D., Mita, S., Collazo, R., Sitar, Z. & Maria, J.-P. Epitaxial calcium oxide films deposited on gallium nitride surfaces. J. Vac. Sci. Technol. B. 25, 1029–1032 (2007).
doi: 10.1116/1.2710243
Migita, S., Kasai, Y. & Sakai, S. Molecular beam epitaxial growth of sro and cao with rheed intensity oscillation. J. Low. Temp. Phys. 105, 1337–1342 (1996).
doi: 10.1007/BF00753886
Hughes, A. E. & Pells, G. P. Absorption and luminescence of bismuth ions implanted into cao and mgo single crystals. Phys. Status Solidi 25, 437–443 (1974).
doi: 10.1002/pssa.2210250209
Swart, H. & Kroon, R. (invited) ultraviolet and visible luminescence from bismuth doped materials. Optical Mater. 2, 100025 (2019).
Armiento, R. Database-Driven High-Throughput Calculations and Machine Learning Models for Materials Design. In Schütt, K. T. et al. (eds) Machine Learning Meets Quantum Physics, vol. 968 of Lecture Notes in Physics (Springer International Publishing, Cham, 2020).
Sharma, P., Verma, S., Jain, A. & Kaurav, N. Theoretical analysis of the structural phase transition in alkaline earth oxides. AIP Conf. Proc. 2100, 020119 (2019).
doi: 10.1063/1.5098673
Lany, S. & Zunger, A. Assessment of correction methods for the band-gap problem and for finite-size effects in supercell defect calculations: Case studies for zno and gaas. Phys. Rev. B 78, 235104 (2008).
doi: 10.1103/PhysRevB.78.235104
Kresse, G. & Hafner, J. Ab initio molecular-dynamics simulation of the liquid-metal-amorphous-semiconductor transition in germanium. Phys. Rev. B 49, 14251–14269 (1994).
doi: 10.1103/PhysRevB.49.14251
Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169–11186 (1996).
doi: 10.1103/PhysRevB.54.11169
Blöchl, P. E. Projector augmented-wave method. Phys. Rev. B 50, 17953–17979 (1994).
doi: 10.1103/PhysRevB.50.17953
Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).
doi: 10.1103/PhysRevB.59.1758
Heyd, J., Scuseria, G. E. & Ernzerhof, M. Hybrid functionals based on a screened coulomb potential. J. Chem. Phys. 118, 8207 (2003).
doi: 10.1063/1.1564060
Heyd, J., Scuseria, G. E. & Ernzerhof, M. Erratum: “hybrid functionals based on a screened coulomb potential” [j. chem. phys. 118, 8207 (2003)]. J. Chem. Phys. 124, 219906 (2006).
doi: 10.1063/1.2204597
Yang, J., Falletta, S. & Pasquarello, A. One-shot approach for enforcing piecewise linearity on hybrid functionals: Application to band gap predictions. J. Phys. Chem. Lett. 13, 3066–3071 (2022).
pubmed: 35352960
doi: 10.1021/acs.jpclett.2c00414
Kaduk, B., Kowalczyk, T. & Van Voorhis, T. Constrained density functional theory. Chem. Rev. 112, 321–370 (2012).
pubmed: 22077560
doi: 10.1021/cr200148b
Davidsson, J. Theoretical polarization of zero phonon lines in point defects. J. Phys. Condens. Matter 32, 385502 (2020).
doi: 10.1088/1361-648X/ab94f4
Govoni, M. & Galli, G. Large Scale GW Calculations. J. Chem. Theory Comput. 11, 2680–2696 (2015).
pubmed: 26575564
doi: 10.1021/ct500958p
Yang, W. & Liu, R.-B. Quantum many-body theory of qubit decoherence in a finite-size spin bath. Phys. Rev. B 78, 085315 (2008).
doi: 10.1103/PhysRevB.78.085315
Yang, W. & Liu, R.-B. Quantum many-body theory of qubit decoherence in a finite-size spin bath. ii. ensemble dynamics. Phys. Rev. B 79, 115320 (2009).
doi: 10.1103/PhysRevB.79.115320
Balian, S. J., Liu, R.-B. & Monteiro, T. S. Keeping a spin qubit alive in natural silicon: Comparing optimal working points and dynamical decoupling. Phys. Rev. B 91, 245416 (2015).
doi: 10.1103/PhysRevB.91.245416
Ma, W.-L., Wolfowicz, G., Li, S.-S., Morton, J. J. L. & Liu, R.-B. Classical nature of nuclear spin noise near clock transitions of bi donors in silicon. Phys. Rev. B 92, 161403 (2015).
doi: 10.1103/PhysRevB.92.161403
Haynes, W. M., Lide, D. R. & Bruno, T. J. CRC handbook of chemistry and physics, 95th ed. (CRC press, 2016).