# First-principles prediction of potentials and space-charge layers in all-solid-state batteries

## TL;DR

This paper develops a first-principles model to predict potential profiles and space-charge layers in all-solid-state batteries, providing insights into their operation and factors influencing performance.

## Contribution

It introduces a fully first-principles-informed model for potential profiles in SSBs, applied to the Li/LiPON/Li_xCoO_2 system, revealing key interfacial phenomena.

## Key findings

- Interfacial potential drops are driven by electron transfer and Li+ space-charge layers.
- Lower electronic ionization potential in electrolyte enhances Li+ transport.
- Model predicts potential variations with state of charge in SSBs.

## Abstract

As all-solid-state batteries (SSBs) develop as an alternative to traditional cells, a thorough theoretical understanding of driving forces behind battery operation is needed. We present a fully first-principles-informed model of potential profiles in SSBs and apply the model to the Li/LiPON/$\text{Li}_x\text{CoO}_2$ system. The model predicts interfacial potential drops driven by both electron transfer and Li$^+$ space-charge layers that vary with the SSB's state of charge. The results suggest lower electronic ionization potential in the solid electrolyte favors Li$^+$ transport, leading to higher discharge power.