Carlos first came to prominence in 1968 with Switched-On Bach, a recording of music by J.S. Bach painstakingly assembled, phrase-by-phrase, on the Moog synthesizer, at the time a relatively new and unknown instrument. The album earned three Grammy Awards in 1969. Other classical recordings followed. Carlos later began releasing original compositions, including the first-ever album of synthesized environmental sounds, Sonic Seasonings (1972) and an album exploring alternate tunings Beauty in the Beast (1986). She has also worked in film music, notably writing and performing scores for two Stanley Kubrick movies, A Clockwork Orange (1971) and The Shining (1980), as well as Walt Disney's Tron (1982).
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