Obviously I don't actually expect a definite answer to this, but I noticed a few times throughout Dawnguard's questline that Serana would mention whoever was in the castle before she and her parents moved in (mentioning the jetty, Valerica replacing the sundial with a moondial, etc). I dunno if it's anything resembling a clue, but I did notice a partially destroyed statue to Mara in part of the ruins, which seems like a weird thing for a bunch of vampires to have, especially Harkon.
But just thought it might be an interesting thread to toss ideas around. What do you think?