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Personally, I would choose two names from a piece of literature. That way the twins wouldn't be burdened with "rhyming names" or anything like that, but still connect in some way.

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Examples:
Morgan and Gwen (Arthurian legend)
Juliet and Rosalind (Romeo and Juliet)
Tom and Finn (The Adventures of Tom Sawyer and Huckleberry Finn)
Sara and Emily (A Little Princess)
Anna and Karenina (Anna Karenina)

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