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I’ve always thought that the stories of Syd de-tuning his guitar onstage, playing on chord over and over and over, were people’s attempts at describing his trying to achieve a pure synthetic sound on his guitar. This has been called “Ambient” too.
Barrett might have been attempting to take his sound “all the way out” and left his band mates scratching their heads. He might have been seeking a pure/new sound not based in Western music or even by playing notes.
For sure, I see Syd Barrett as a precursor to Robert Fripp and that whole universe that he helped open up.
Here are some examples of groups trying something similar at the same time as Syd:
Red Crayola - Boards 1967:
Velvet Underground - Melody Laughter 1966:
Mothers - The Return of the Son of the Monster Magnet 1966: