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PreprintCC BY 4.0arXiv

Direct observation of reversible ionic polarization at a buried solid-state battery interface

Abstract

Electric fields control ionic distributions at solid-solid interfaces. However, whether buried interfaces possess an intrinsic ionic reversibility has remained experimentally unresolved. Here, we directly observe reversible ionic polarization at the buried amorphous LiCoO2/Li1.5Al0.5Ge1.5P3O12 electrolyte interface. By combining the Elastic Recoil Detection Analysis (ERDA) method, utilizing time-of-flight (ToF) measurements and nanometer-scale resolution, with the Neutron Depth Profiling (NDP) method for the absolute quantification of lithium, we show that an applied bias of +-1 V results in a reversible redistribution of approximately 9.3% of lithium in the interface region, while conserving its total content. Upon polarity reversal, the lithium redistribution is completely reversed, indicating reversible interfacial ionic polarization rather than irreversible lithium loss or permanent interphase formation. These results demonstrate that buried interfaces in solidelectrolyte systems can behave as electrically reconfigurable ionic regions with an intrinsic reversible freedom for ion motion, thereby providing direct microscopic insight into the physics of space-charge formation and low-voltage interfacial response in solid-state electrochemical systems.

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BibTeX
@misc{ceccio2026direct,
  title = {{Direct observation of reversible ionic polarization at a buried solid-state battery interface}},
  author = {Giovanni Ceccio and Romana Miksova and Jiri Vacik and Zoltan Szaraz and Josef Dobrovodsky and Pavlina Zavadilová and Pavol Noga and Ivan Mastronardo},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.12626},
  eprint = {2609.12626},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.12626},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - Direct observation of reversible ionic polarization at a buried solid-state battery interface
AU  - Giovanni Ceccio
AU  - Romana Miksova
AU  - Jiri Vacik
AU  - Zoltan Szaraz
AU  - Josef Dobrovodsky
AU  - Pavlina Zavadilová
AU  - Pavol Noga
AU  - Ivan Mastronardo
PY  - 2026
DA  - 2026/09/11
PB  - arXiv
DO  - 10.48550/arxiv.2609.12626
UR  - https://arxiv.org/abs/2609.12626
AB  - Electric fields control ionic distributions at solid-solid interfaces. However, whether buried interfaces possess an intrinsic ionic reversibility has remained experimentally unresolved. Here, we directly observe reversible ionic polarization at the buried amorphous LiCoO2/Li1.5Al0.5Ge1.5P3O12 electrolyte interface. By combining the Elastic Recoil Detection Analysis (ERDA) method, utilizing time-of-flight (ToF) measurements and nanometer-scale resolution, with the Neutron Depth Profiling (NDP) method for the absolute quantification of lithium, we show that an applied bias of +-1 V results in a reversible redistribution of approximately 9.3% of lithium in the interface region, while conserving its total content. Upon polarity reversal, the lithium redistribution is completely reversed, indicating reversible interfacial ionic polarization rather than irreversible lithium loss or permanent interphase formation. These results demonstrate that buried interfaces in solidelectrolyte systems can behave as electrically reconfigurable ionic regions with an intrinsic reversible freedom for ion motion, thereby providing direct microscopic insight into the physics of space-charge formation and low-voltage interfacial response in solid-state electrochemical systems.
ER  -