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Is it correct to say "You which know the secret of my heart"? If yes, what is the difference from "You who know .... " ?

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No, it's not correct to say "you which know". Your second sentence, "you who know", is OK, but clumsy.

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Thank you very much for your help. How could I express the sentence : "You WHO know the secrets of my heart, give me a shining smile, one more time" in a better way? It's a song... Thanks! – Simone Pacchioni May 30 '13 at 13:50
In a song, it's OK. But nobody talks like that. Normally relative clauses do not modify pronouns -- relative clauses are to identify nouns, and pronouns are for nouns that are already identified. – John Lawler May 30 '13 at 13:55
you THAT now? better or not than you WHO know? – Simone Pacchioni Jun 5 '13 at 14:31

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