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Main Authors: Sperlich, Andreas, Eckstein, Klaus H., Oberndorfer, Florian, Sturzda, Bernd K., Auth, Michael, Dyakonov, Vladimir, Mitric, Roland, Hertel, Tobias
Format: Preprint
Published: 2024
Subjects:
Online Access:https://arxiv.org/abs/2403.05361
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author Sperlich, Andreas
Eckstein, Klaus H.
Oberndorfer, Florian
Sturzda, Bernd K.
Auth, Michael
Dyakonov, Vladimir
Mitric, Roland
Hertel, Tobias
author_facet Sperlich, Andreas
Eckstein, Klaus H.
Oberndorfer, Florian
Sturzda, Bernd K.
Auth, Michael
Dyakonov, Vladimir
Mitric, Roland
Hertel, Tobias
contents Nanoscale semiconductors with isolated spin impurities have been touted as promising materials for their potential use at the intersection of quantum, spin, and information technologies. Electron paramagnetic resonance (EPR) studies of spins in semiconducting carbon nanotubes have overwhelmingly focused on spins more strongly localized by $\rm sp^3$-type lattice defects. However, the creation of such impurities is irreversible and requires specific reactions to generate them. Shallow charge impurities, on the other hand, are more readily and widely produced by simple redox chemistry, but have not yet been investigated for their spin properties. Here we use EPR to study p-doped (6,5) semiconducting single-wall carbon nanotubes (s-SWNTs) and elucidate the role of impurity-impurity interactions in conjunction with exchange and correlation effects for the spin behavior of this material. A quantitative comparison of the EPR signals with phenomenological modeling combined with configuration interaction electronic structure calculations of impurity pairs shows that orbital overlap, combined with exchange and correlation effects, causes the EPR signal to disappear due to spin entanglement for doping levels corresponding to impurity spacings of $14\,\rm nm$ (at 30 K). This transition is predicted to shift to higher doping levels with increasing temperature and to lower levels with increasing screening, providing an opportunity for improved spin control in doped s-SWNTs.
format Preprint
id arxiv_https___arxiv_org_abs_2403_05361
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Onset of Spin Entanglement in Doped Carbon Nanotubes Studied by EPR
Sperlich, Andreas
Eckstein, Klaus H.
Oberndorfer, Florian
Sturzda, Bernd K.
Auth, Michael
Dyakonov, Vladimir
Mitric, Roland
Hertel, Tobias
Materials Science
Nanoscale semiconductors with isolated spin impurities have been touted as promising materials for their potential use at the intersection of quantum, spin, and information technologies. Electron paramagnetic resonance (EPR) studies of spins in semiconducting carbon nanotubes have overwhelmingly focused on spins more strongly localized by $\rm sp^3$-type lattice defects. However, the creation of such impurities is irreversible and requires specific reactions to generate them. Shallow charge impurities, on the other hand, are more readily and widely produced by simple redox chemistry, but have not yet been investigated for their spin properties. Here we use EPR to study p-doped (6,5) semiconducting single-wall carbon nanotubes (s-SWNTs) and elucidate the role of impurity-impurity interactions in conjunction with exchange and correlation effects for the spin behavior of this material. A quantitative comparison of the EPR signals with phenomenological modeling combined with configuration interaction electronic structure calculations of impurity pairs shows that orbital overlap, combined with exchange and correlation effects, causes the EPR signal to disappear due to spin entanglement for doping levels corresponding to impurity spacings of $14\,\rm nm$ (at 30 K). This transition is predicted to shift to higher doping levels with increasing temperature and to lower levels with increasing screening, providing an opportunity for improved spin control in doped s-SWNTs.
title Onset of Spin Entanglement in Doped Carbon Nanotubes Studied by EPR
topic Materials Science
url https://arxiv.org/abs/2403.05361