Stability and molecular pathways to the formation of spin defects in silicon carbide

Lee, Elizabeth M. Y.; Yu, Alvin; de Pablo, Juan J.; Galli, Giulia

doi:10.1038/s41467-021-26419-0

Stability and molecular pathways to the formation of spin defects in silicon carbide

Journal Article · Wed Nov 03 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-26419-0· OSTI ID:1829138

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Abstract

Spin defects in wide-bandgap semiconductors provide a promising platform to create qubits for quantum technologies. Their synthesis, however, presents considerable challenges, and the mechanisms responsible for their generation or annihilation are poorly understood. Here, we elucidate spin defect formation processes in a binary crystal for a key qubit candidate—the divacancy complex (VV) in silicon carbide (SiC). Using atomistic models, enhanced sampling simulations, and density functional theory calculations, we find that VV formation is a thermally activated process that competes with the conversion of silicon (V _Si ) to carbon monovacancies (V _C ), and that VV reorientation can occur without dissociation. We also find that increasing the concentration of V _Si relative to V _C favors the formation of divacancies. Moreover, we identify pathways to create spin defects consisting of antisite-double vacancy complexes and determine their electronic properties. The detailed view of the mechanisms that underpin the formation and dynamics of spin defects presented here may facilitate the realization of qubits in an industrially relevant material.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Midwest Integrated Center for Computational Materials (MICCoM); National Institutes of Health (NIH); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1829138

Alternate ID(s):: OSTI ID: 1868930

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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