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C. Polop

Publications and source records attributed to C. Polop.

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Nanoscale imaging reveals critical plating and stripping mechanisms in anode-free lithium and sodium solid-state batteries

Achieving reversible anode-free solid-state batteries hinges on controlling alkali-metal plating and stripping at buried interfaces, yet the underlying nanoscale mechanisms remain unresolved. Here we introduce virtual-electrode low-energy electron microscopy (VE-LEEM), an imaging platform that enables nanoscale visualization of anode formation and dissolution by combining electron beam-induced plating with ultraviolet-driven stripping. By integrating VE LEEM with synchrotron-based photoemission electron microscopy and atomic force microscopy, we track the chemical and morphological evolution of Li and Na anodes during cycling. We uncover a shared dynamic scaling regime governing anode growth, analogous to high mobility thin film deposition, but emerging through distinct morphological pathways dictated by metal-specific surface energetics. This universal scaling behaviour establishes a transferable quantitative framework for comparing anode-free plating across chemistries. In contrast, stripping proceeds through sequential grain-boundary unzipping and cluster decay mechanisms, demonstrating that dissolution is intrinsically asymmetric with respect to plating and leaves behind a persistent interfacial residual layer. These results overturn the common assumption of mirrored plating-stripping dynamics and identify interfacial and grain boundary energetics as fundamental constraints on reversibility. VE LEEM thus provides a general route to resolve buried electrochemical interfaces at the nanoscale and establishes an energetic framework to guide the design of durable, high energy anode free solid state batteries.

cond-mat.mtrl-sci

A multi-technique approach to understanding delithiation damage in LiCoO2 thin films

We report on the delithiation of LiCoO2 thin films using oxalic acid (C2H2O4) with the goal of understanding the structural degradation of an insertion oxide associated with Li chemical extraction. Using a multi-technique approach that includes synchrotron radiation x-ray diffraction, scanning electron microscopy, micro Raman spectroscopy, photoelectron spectroscopy and conductive atomic force microscopy we reveal the balance between selective Li extraction and structural damage. We identify three different delithiation regimes, related to surface processes, bulk delithiation and damage generation. We find that only a fraction of the grains is affected by the delithiation process, which may create local inhomogeneities. The chemical route to Li extraction provides additional opportunities to investigate delithiation while avoiding the complications associated with electrolyte breakdown and could simplify in situ measurements.

cond-mat.mtrl-sci