He composed most of the material for Piper at the Gates of dawn and contributed a couple of songs to Saucerful of secrets.
He had a bit of a nervous breakdown after taking one too many acid trips which was compounded by the fact that he had Aspergers Syndrome. The other members kicked him out of the band when he became too mentally unstable and difficult to deal with.
He was a very underrated songwriter before his breakdown. Piper at the Gates of Dawn is an amazing album.