The part that sealed his role was when he asked Arwen if he also did not have her love. Right then, you see some of the "harshness" slip away and see a very caring father worried for his daughters fate. A sort of helpless look, like he knows he can't make her go but he wishes that he could. It's quick and subtle, but it's there. Hugo did such a good job with that scene I'm almost willing to forget how 2-D Elrond's movie character was written.
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"Don't Panic."
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