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ToF-SIMS Li Depth Profiling of Pure and Methylated Amorphous Silicon Electrodes After Their Partial Lithiation.

Pure (a-Si:H) and methylated [a-Si0.95(CH3)0.05:H] amorphous silicon thin films were analyzed by time-of-flight secondary ion mass spectrometry after partial lithiation. Depth profiling gives insights into the lithiation mechanism of the material, enabling us to study the detailed biphasic process in the first lithiation process. Lithiation induces swelling and roughening of the active layer. In both a-Si:H and a-Si0.95(CH3)0.05:H, no measurable Li diffusion was observed after stopping current-induced lithiation. After applying the same lithiation charges, distinct Li profiles were observed for these two materials. Unlike a-Si:H, the Li concentration drops slowly from the heavily lithiated region to the non-lithiated region in a-Si0.95(CH3)0.05:H. This apparent progressive transition between the lithiated and lithium-free regions is attributed to the presence of nanovoids inside the material. When their concentration is high enough, these nanovoids constitute favorable quasi-percolating paths for lithium during the first lithiation. A specific model was developed to simulate the Li depth profiles, fully supporting this hypothesis.