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A really good band that a Japanese exchange student friend sent me a bunch of songs from is Love Psychedelico (which I hoped I spelled right). Their stuff kind of ranges but it's mostly a kind of relaxed electronic/alternative kind of vibe.
I don't know how popular or accessible their songs might be for download, etc because a lot of the bands he sent me are ones that are indie or non-mainstream but try to find a few of theirs because it's pretty good.
You've probably heard it already but the Hellsing soundtrack is also nice. I'm not sure if it was done by an established band or someone composing specifically for the anime but it's good.
Also, the pillows are (I'm almost positive) a band and not just assembled for the sake of the FLCL soundtrack. Their career might have only lasted for that show though so that may be the only released material.
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