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Title: Probing long-range carrier-pair spin–spin interactions in a conjugated polymer by detuning of electrically detected spin beating

Abstract

Here, weakly coupled electron spin pairs that experience weak spin–orbit interaction can control electronic transitions in molecular and solid-state systems. Known to determine radical pair reactions, they have been invoked to explain phenomena ranging from avian magnetoreception to spin-dependent charge-carrier recombination and transport. Spin pairs exhibit persistent spin coherence, allowing minute magnetic fields to perturb spin precession and thus recombination rates and photoreaction yields, giving rise to a range of magneto-optoelectronic effects in devices. Little is known, however, about interparticle magnetic interactions within such pairs. Here we present pulsed electrically detected electron spin resonance experiments on poly(styrene-sulfonate)-doped poly(3,4-ethylenedioxythiophene) (PEDOT:PSS) devices, which show how interparticle spin–spin interactions (magnetic-dipolar and spin-exchange) between charge-carrier spin pairs can be probed through the detuning of spin-Rabi oscillations. The deviation from uncoupled precession frequencies quantifies both the exchange (<30 neV) and dipolar (23.5±1.5 neV) interaction energies responsible for the pair’s zero-field splitting, implying quantum mechanical entanglement of charge-carrier spins over distances of 2.1±0.1 nm.

Authors:
 [1];  [1];  [1];  [2];  [1]
  1. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Physics and Astronomy
  2. Univ. of Utah, Salt Lake City, UT (United States). Dept. of Physics and Astronomy; Univ. of Regensburg, Regensburg (Germany). Inst. of Experimental and Applied Physics
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1454251
Grant/Contract Number:  
SC0000909
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

van Schooten, Kipp J., Baird, Douglas L., Limes, Mark E., Lupton, John M., and Boehme, Christoph. Probing long-range carrier-pair spin–spin interactions in a conjugated polymer by detuning of electrically detected spin beating. United States: N. p., 2015. Web. doi:10.1038/ncomms7688.
van Schooten, Kipp J., Baird, Douglas L., Limes, Mark E., Lupton, John M., & Boehme, Christoph. Probing long-range carrier-pair spin–spin interactions in a conjugated polymer by detuning of electrically detected spin beating. United States. doi:10.1038/ncomms7688.
van Schooten, Kipp J., Baird, Douglas L., Limes, Mark E., Lupton, John M., and Boehme, Christoph. Tue . "Probing long-range carrier-pair spin–spin interactions in a conjugated polymer by detuning of electrically detected spin beating". United States. doi:10.1038/ncomms7688. https://www.osti.gov/servlets/purl/1454251.
@article{osti_1454251,
title = {Probing long-range carrier-pair spin–spin interactions in a conjugated polymer by detuning of electrically detected spin beating},
author = {van Schooten, Kipp J. and Baird, Douglas L. and Limes, Mark E. and Lupton, John M. and Boehme, Christoph},
abstractNote = {Here, weakly coupled electron spin pairs that experience weak spin–orbit interaction can control electronic transitions in molecular and solid-state systems. Known to determine radical pair reactions, they have been invoked to explain phenomena ranging from avian magnetoreception to spin-dependent charge-carrier recombination and transport. Spin pairs exhibit persistent spin coherence, allowing minute magnetic fields to perturb spin precession and thus recombination rates and photoreaction yields, giving rise to a range of magneto-optoelectronic effects in devices. Little is known, however, about interparticle magnetic interactions within such pairs. Here we present pulsed electrically detected electron spin resonance experiments on poly(styrene-sulfonate)-doped poly(3,4-ethylenedioxythiophene) (PEDOT:PSS) devices, which show how interparticle spin–spin interactions (magnetic-dipolar and spin-exchange) between charge-carrier spin pairs can be probed through the detuning of spin-Rabi oscillations. The deviation from uncoupled precession frequencies quantifies both the exchange (<30 neV) and dipolar (23.5±1.5 neV) interaction energies responsible for the pair’s zero-field splitting, implying quantum mechanical entanglement of charge-carrier spins over distances of 2.1±0.1 nm.},
doi = {10.1038/ncomms7688},
journal = {Nature Communications},
number = 1,
volume = 6,
place = {United States},
year = {2015},
month = {4}
}

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Cited by: 23 works
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Works referenced in this record:

Transport properties of poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate)
journal, April 1998


Hyperfine-Field-Mediated Spin Beating in Electrostatically Bound Charge Carrier Pairs
journal, January 2010

  • McCamey, D. R.; van Schooten, K. J.; Baker, W. J.
  • Physical Review Letters, Vol. 104, Issue 1, Article No. 017601
  • DOI: 10.1103/PhysRevLett.104.017601