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<p>Space-charge layers (SCLs) at heterogeneous interfaces generate electrostatic potential drops that can enhance or impede ionic and electronic transport near the interface. In solid-state Li-ion batteries, previous models typically only consider Li-ions as the mobile defect, even though cations, anions, and electrons can all participate in SCL formation. Here, we introduce a general first-principles defect-based framework to quantify these multi-species contributions and apply it to LiPON/Li<sub><i>x</i></sub>V<sub>2</sub>O<sub>5</sub> interfaces (<i>x</i> = 0, 1, 2 for the alpha, delta, and gamma phases). A systematic screening of charged point defect formation energies identified Li-ion vacancies, Li-ion interstitials, and O-ion vacancies as dominant species. The model reveals spontaneous Li-ion transfer from LiPON into Li<sub><i>x</i></sub>V<sub>2</sub>O<sub>5</sub> and O-species transfer in the opposite direction, behaviors missed by Li-only treatments. Band alignments across the interfaces show electrons initially transferring from LiPON into V<sub>2</sub>O<sub>5</sub>, however, when the lithium content increases in Li<sub><i>x</i></sub>V<sub>2</sub>O<sub>5</sub>, the direction of electron transfer reverses. Consequently, the predicted band-bending switches from downward bending in V<sub>2</sub>O<sub>5</sub> to upward bending in the LiV<sub>2</sub>O<sub>5</sub> and Li<sub>2</sub>V<sub>2</sub>O<sub>5</sub> phases. The implications of these SCL-induced potentials for Li-ion and electron transport are discussed for solid-state batteries and electrochemical neuromorphic devices, highlighting the importance of explicitly accounting for multi-ion defect transfer.</p>

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Multi-ion defect model for space-charge layer formation at LiPON/LixV2O5 electrochemical interfaces

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月19日

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  • Gregory Pustorino,
  • Leopoldo Jose Tapia-Aracayo,
  • Daniel Halbing,
  • Leonard Brillson,
  • David Stewart,
  • Yue Qi

摘要

Space-charge layers (SCLs) at heterogeneous interfaces generate electrostatic potential drops that can enhance or impede ionic and electronic transport near the interface. In solid-state Li-ion batteries, previous models typically only consider Li-ions as the mobile defect, even though cations, anions, and electrons can all participate in SCL formation. Here, we introduce a general first-principles defect-based framework to quantify these multi-species contributions and apply it to LiPON/LixV2O5 interfaces (x = 0, 1, 2 for the alpha, delta, and gamma phases). A systematic screening of charged point defect formation energies identified Li-ion vacancies, Li-ion interstitials, and O-ion vacancies as dominant species. The model reveals spontaneous Li-ion transfer from LiPON into LixV2O5 and O-species transfer in the opposite direction, behaviors missed by Li-only treatments. Band alignments across the interfaces show electrons initially transferring from LiPON into V2O5, however, when the lithium content increases in LixV2O5, the direction of electron transfer reverses. Consequently, the predicted band-bending switches from downward bending in V2O5 to upward bending in the LiV2O5 and Li2V2O5 phases. The implications of these SCL-induced potentials for Li-ion and electron transport are discussed for solid-state batteries and electrochemical neuromorphic devices, highlighting the importance of explicitly accounting for multi-ion defect transfer.