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Title: Spin Signature of the C 60 Fullerene Anion: A Combined X- and D-Band EPR and DFT Study

Abstract

Fullerenes attract much attention in various scientific fields, but their electronic properties are still not completely understood. Here we report on a combined EPR and DFT study of the fullerene anion C 60 in solid glassy environment. DFT calculations were used to characterize its electronic structure through spin density distribution and magnetic resonance parameters. The electron spin density is not uniformly distributed throughout the C 60 cage but shows a pattern similar to PC 61BM . EPR spectroscopy reveals a rhombic g-tensor sensitive to the environment in the frozen glassy solutions, which can be rationalized by deformation of the fullerenes along lowfrequency vibrational modes upon cooling. DFT modeling confirms that these deformations lead to variation in the C 60 g values. Furthermore, the decrease in g-tensor anisotropy with sample annealing is related to the lessening of g-tensor strain upon temperature relaxation of the most distorted sites in the glassy state.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Chicago State Univ., Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1476900
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 14; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; C60; DFT; Density Functional Theory; EPR; Electron Paramagnetic Resonance; Fullerene; PC61BM; Radical Anion; g-tensor

Citation Formats

Niklas, Jens, Mardis, Kristy L., and Poluektov, Oleg G. Spin Signature of the C60 Fullerene Anion: A Combined X- and D-Band EPR and DFT Study. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b01613.
Niklas, Jens, Mardis, Kristy L., & Poluektov, Oleg G. Spin Signature of the C60 Fullerene Anion: A Combined X- and D-Band EPR and DFT Study. United States. doi:10.1021/acs.jpclett.8b01613.
Niklas, Jens, Mardis, Kristy L., and Poluektov, Oleg G. Tue . "Spin Signature of the C60 Fullerene Anion: A Combined X- and D-Band EPR and DFT Study". United States. doi:10.1021/acs.jpclett.8b01613. https://www.osti.gov/servlets/purl/1476900.
@article{osti_1476900,
title = {Spin Signature of the C60 Fullerene Anion: A Combined X- and D-Band EPR and DFT Study},
author = {Niklas, Jens and Mardis, Kristy L. and Poluektov, Oleg G.},
abstractNote = {Fullerenes attract much attention in various scientific fields, but their electronic properties are still not completely understood. Here we report on a combined EPR and DFT study of the fullerene anion C60– in solid glassy environment. DFT calculations were used to characterize its electronic structure through spin density distribution and magnetic resonance parameters. The electron spin density is not uniformly distributed throughout the C60– cage but shows a pattern similar to PC61BM–. EPR spectroscopy reveals a rhombic g-tensor sensitive to the environment in the frozen glassy solutions, which can be rationalized by deformation of the fullerenes along lowfrequency vibrational modes upon cooling. DFT modeling confirms that these deformations lead to variation in the C60– g values. Furthermore, the decrease in g-tensor anisotropy with sample annealing is related to the lessening of g-tensor strain upon temperature relaxation of the most distorted sites in the glassy state.},
doi = {10.1021/acs.jpclett.8b01613},
journal = {Journal of Physical Chemistry Letters},
number = 14,
volume = 9,
place = {United States},
year = {2018},
month = {7}
}

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