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Title: Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering

Here, we discuss how x-ray Compton scattering spectra can be used for investigating the evolution of electronic states in cathode materials of Li batteries under the lithiation/delithiation process. In particular, our analysis of the Compton spectra taken from polycrystalline Li xCoO 2 samples shows that the spectra are dominated by the contribution of the O-2p redox orbital. We identify a distinct signature of d-orbital delocalization, which is tied directly to the conductivity of the material, providing a descriptor based on Compton spectra for monitoring the lithiation range with improved conductivity and kinetics for electrochemical operation. Our study demonstrates that Compton scattering spectroscopy can provide a window for probing complex electronic mechanisms underlying the charging and discharging processes in Li-battery materials.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [3] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [5] ;  [2]
  1. Northeastern Univ., Boston, MA (United States). Dept. of Physics
  2. Gunma Univ. (Japan). Faculty of Science and Technology
  3. Kyoto Univ. (Japan). Guraduate School of Human and Environmental Studies
  4. Northeastern Univ., Boston, MA (United States). Dept. of Physics; AGH - Univ. of Science and Technology, Krakow (Poland). Faculty of Physics and Applied Computer Science
  5. Japan Synchrotron Radiation Research Inst. (JASRI), Hyogo (Japan)
Publication Date:
Grant/Contract Number:
FG02-07ER46352; AC02-05CH11231; 24750065; 15K17873; 2013B1187
Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 109; Journal Issue: 7; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Research Org:
Northeastern Univ., Boston, MA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Japan Science and Technology Agency (JST); Ministry of Education, Culture, Sports, Science and Technology (MEXT)
Contributing Orgs:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; redox; electrons; electron transfer; batteries; cathodes; lithium; wave functions; compton scattering
OSTI Identifier:
1467864
Alternate Identifier(s):
OSTI ID: 1294704

Barbiellini, B., Suzuki, K., Orikasa, Y., Kaprzyk, S., Itou, M., Yamamoto, K., Wang, Yung Jui, Hafiz, H., Yamada, R., Uchimoto, Y., Bansil, A., Sakurai, Y., and Sakurai, H.. Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering. United States: N. p., Web. doi:10.1063/1.4961055.
Barbiellini, B., Suzuki, K., Orikasa, Y., Kaprzyk, S., Itou, M., Yamamoto, K., Wang, Yung Jui, Hafiz, H., Yamada, R., Uchimoto, Y., Bansil, A., Sakurai, Y., & Sakurai, H.. Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering. United States. doi:10.1063/1.4961055.
Barbiellini, B., Suzuki, K., Orikasa, Y., Kaprzyk, S., Itou, M., Yamamoto, K., Wang, Yung Jui, Hafiz, H., Yamada, R., Uchimoto, Y., Bansil, A., Sakurai, Y., and Sakurai, H.. 2016. "Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering". United States. doi:10.1063/1.4961055. https://www.osti.gov/servlets/purl/1467864.
@article{osti_1467864,
title = {Identifying a descriptor for d-orbital delocalization in cathodes of Li batteries based on x-ray Compton scattering},
author = {Barbiellini, B. and Suzuki, K. and Orikasa, Y. and Kaprzyk, S. and Itou, M. and Yamamoto, K. and Wang, Yung Jui and Hafiz, H. and Yamada, R. and Uchimoto, Y. and Bansil, A. and Sakurai, Y. and Sakurai, H.},
abstractNote = {Here, we discuss how x-ray Compton scattering spectra can be used for investigating the evolution of electronic states in cathode materials of Li batteries under the lithiation/delithiation process. In particular, our analysis of the Compton spectra taken from polycrystalline LixCoO2 samples shows that the spectra are dominated by the contribution of the O-2p redox orbital. We identify a distinct signature of d-orbital delocalization, which is tied directly to the conductivity of the material, providing a descriptor based on Compton spectra for monitoring the lithiation range with improved conductivity and kinetics for electrochemical operation. Our study demonstrates that Compton scattering spectroscopy can provide a window for probing complex electronic mechanisms underlying the charging and discharging processes in Li-battery materials.},
doi = {10.1063/1.4961055},
journal = {Applied Physics Letters},
number = 7,
volume = 109,
place = {United States},
year = {2016},
month = {8}
}