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Metal‐catalyzed asymmetric alkylation of indoles with α‐diazoesters is well‐known, however, the underlying mechanisms of this reaction, particularly the origin of stereoselectivity, remain uncertain. For the Pd catalysis, we address this cutting‐edge challenge from two complementary viewpoints – i) the molecular level regarding a single catalytically active Pd center; and ii) nano‐level Pd species...
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