Yeah 'Subbacultcha' is definely one of the album's best moments. It's not my favourite version of that song though. I think the song sounds better in rawer form like on Pixies At The BBC and 'The Purple Album', it seems to have more urgency and purpose.
He was heading into new musical territories but really he could only do it on his own and for that he had to either take full creative control of the band or go it alone. The former wasn't going to work out, especially with Kim Deal who had her own band The Breeders, so the band split and he went solo.
I think the band peaked with Doolittle but even by that time I think they had matured somewhat from the chaos of Come On Pilgrim and Surfer Rosa. I think you're right about Black Francis not taking himself too seriously as a musician especially in the early days of the band. It was all pretty much tongue-in-cheek and a crazy sense of humour, they were enjoying themselves as a band as well and just playing around with ideas.
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