Well, that one has most of the tracks from all three previous albums. Clearly, that's better value, but the downsides are that it could be overkill plus it strangely omits a key track from Souvlaki (When The Sun Hits) which is many people's favourite track. However, it's a fairly extensive compilation. I don't think you'll like the tracks from Pygmalion that much - they're like a guitar-based version of electronica with some elements of dub. If you want to keep it pure, go for Souvlaki; if you go for this one, be selective with the tracks or you may find it a bit "Meh" - there are some of their least interesting songs on that compilation.
You need When The Sun Hits. Just saying
Thanks.
I think.