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Probing Electron Transfer Orbitals Selectively at LiCoO2/C Cathode Interfaces via Positron Annihilation Spectroscopy

Meiying Zheng1,2,*, Jan Kuriplach3, Ilja Makkonen4, Rafael Ferragut1,2,5,†, Ekaterina Laakso2, Gioele Pagot6, Vito Di Noto6, and Bernardo Barbiellini2,7,8,‡

  • 1L-NESS and Department of Physics, Politecnico di Milano, Via Anzani 42, IT-22100, Como, Italy
  • 2LUT School of Engineering Sciences, LUT University, Yliopistonkatu 34, FI-53850, Lappeenranta, Finland
  • 3Department of Low Temperature Physics, Faculty of Mathematics and Physics, Charles University, V Holešovičkách 2, CZ-18000, Prague, Czech Republic
  • 4Department of Physics, University of Helsinki, P.O. Box 43, FI-00014, Helsinki, Finland
  • 5INFN Milano unit, National Institute for Nuclear Physics, IT-20133, Milano, Italy
  • 6Section of Chemistry for the Technology (ChemTech) and INSTM, Department of Industrial Engineering, University of Padova, Via Marzolo 9, IT-35131, Padova, Italy
  • 7Department of Physics, Northeastern University, Boston, Massachusetts 02115, USA
  • 8Quantum Materials and Sensing Institute, Northeastern University, Burlington, Massachusetts 01803, USA

  • *Contact author: meiying.zheng@polimi.it
  • †Contact author: rafael.ferragut@polimi.it
  • ‡Contact author: bernardo.barbiellini@lut.fi
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Phys. Rev. Lett. 136, 096402 – Published 5 March, 2026

DOI: https://doi.org/10.1103/9gfy-lxbp

Abstract

Conductive carbon additives in lithium-ion battery cathodes significantly increase electron transport, facilitating rapid charging. However, quantifying this improvement remains challenging. Momentum distribution of annihilating electron-positron pairs offers a powerful approach to selectively probe the O 2p orbitals in LiCoO2 microparticles and the 2pz carbon orbitals in the conductive carbon additives. By analyzing this momentum distribution, we obtain the amplification of subtle electron momentum distribution signals from carbon π bonds. Ab initio modeling of LiCoO2 and various topologies of carbon structures reproducing the experimental momentum distribution helps to quantify the fraction of positron annihilation occurring within the carbon structures. Our theoretical results combined with earlier experimental findings reveal potential charge transport pathways in the LiCoO2/C composite by quantifying the spectral contributions of electron transfer orbitals, which constitutes the nanoscale circuitry enabling efficient electron transport in battery cathodes.

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Phys. Rev. Lett. 136, 096402– Published 5 March, 2026
  • Received 20 October 2024
  • Revised 9 May 2025
  • Accepted 20 January 2026
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