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Despite recent advances in characterising the properties of mature \u03b1S fibrils, the transient and heterogeneous intermediates that underlie cellular toxicity remain largely elusive. Here, we review the mechanistic principles of \u03b1S aggregation, focussing on liquid\u2013liquid phase separation (LLPS) as a critical intermediate step. We discuss how the structural evolution of \u03b1S within the condensed phase governs the subsequent patterns of cellular dysfunction and pathological propagation. 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