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 sp3-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 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.
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14 June 2024
Research Article|
June 17 2024
Onset of spin entanglement in doped carbon nanotubes studied by EPR
Special Collection:
Festschrift in honor of Louis E. Brus
Andreas Sperlich
;
Andreas Sperlich
(Conceptualization, Data curation, Formal analysis, Funding acquisition, Investigation, Methodology, Project administration, Resources, Supervision, Visualization, Writing – original draft, Writing – review & editing)
1
Experimental Physics 6 and Würzburg-Dresden Cluster of Excellence ct.qmat, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Klaus H. Eckstein
;
Klaus H. Eckstein
(Data curation, Formal analysis, Investigation, Visualization, Writing – original draft, Writing – review & editing)
2
Institute of Physical and Theoretical Chemistry, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Florian Oberndorfer;
Florian Oberndorfer
(Data curation, Formal analysis, Investigation, Writing – review & editing)
2
Institute of Physical and Theoretical Chemistry, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Bernd K. Sturdza
;
Bernd K. Sturdza
(Data curation, Formal analysis, Investigation)
1
Experimental Physics 6 and Würzburg-Dresden Cluster of Excellence ct.qmat, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Michael Auth
;
Michael Auth
(Data curation, Formal analysis, Investigation, Visualization, Writing – original draft)
1
Experimental Physics 6 and Würzburg-Dresden Cluster of Excellence ct.qmat, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Vladimir Dyakonov
;
Vladimir Dyakonov
(Conceptualization, Data curation, Formal analysis, Funding acquisition, Investigation, Methodology, Project administration, Resources, Supervision, Visualization, Writing – original draft, Writing – review & editing)
1
Experimental Physics 6 and Würzburg-Dresden Cluster of Excellence ct.qmat, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Roland Mitric
;
Roland Mitric
(Conceptualization, Data curation, Formal analysis, Funding acquisition, Investigation, Methodology, Project administration, Resources, Supervision, Writing – original draft, Writing – review & editing)
2
Institute of Physical and Theoretical Chemistry, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
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Tobias Hertel
Tobias Hertel
a)
(Conceptualization, Data curation, Formal analysis, Funding acquisition, Investigation, Methodology, Project administration, Resources, Supervision, Visualization, Writing – original draft, Writing – review & editing)
2
Institute of Physical and Theoretical Chemistry, Julius-Maximilians-Universität Würzburg
, Würzburg, Germany
a)Author to whom correspondence should be addressed: tobias.hertel@uni-wuerzburg.de
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a)Author to whom correspondence should be addressed: tobias.hertel@uni-wuerzburg.de
J. Chem. Phys. 160, 234702 (2024)
Article history
Received:
March 08 2024
Accepted:
May 14 2024
Citation
Andreas Sperlich, Klaus H. Eckstein, Florian Oberndorfer, Bernd K. Sturdza, Michael Auth, Vladimir Dyakonov, Roland Mitric, Tobias Hertel; Onset of spin entanglement in doped carbon nanotubes studied by EPR. J. Chem. Phys. 14 June 2024; 160 (23): 234702. https://doi.org/10.1063/5.0207502
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