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If you can stand them, I read an article saying that all the string parts on Sigur Ros's "( )" were improvised, but the songs are still structured, so I don't know if that will help you.
There was one album, it's Ornette Coleman and some one else, I forget who, but it was amazing and a free improvisation studio album.
Talk about improvising soundtracks to plays or films. Bring up SYR6 and Sigur Ros's ep "Ba Ba Ti Ki Di Do" which was them and some members of Radiohead improvising the soundtrack to a ballet performance.
Hope I've helped you.
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