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well, moving everything in one go might be way to much work, but imho it'd be good to start small. Firefox 2.0 could go in /usr, KDE 4 could go in /usr, etcetera. Small steps for Archlinux, a big step for cleaning up.
I don't like moving any stuff from /opt to /usr at all. But if the move could happen in some future, then I think it should be only at the same time with major releases of moved software, i.e. Firefox 2.0, KDE 4 (IIRC it will have splitted packages) etc.
to live is to die
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