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He studied keyboard instruments at the Royal College of Music in London from 1938 to 1939, and also studied mathematics at University College, Exeter (B.Sc. 1942). In 1947 he was appointed assistant lecturer in music at the University of Cambridge, subsequently lecturer (1952), and professor (1962). During this time at Cambridge, Dart was the most effective British supporter of the modern early music revival, in part through his influence on those who ultimately formed such groups as the Early Music Consort of London. In 1964 he was appointed King Edward Professor of Music in the University of London (King's College).
As a continuo player he made numerous appearances on the harpsichord, and made many harpsichord, clavichord and organ recordings, especially for the L'Oiseau-Lyre label; he was also a conductor. He served as editor of the Galpin Society Journal from 1947 to 1954 and secretary of Musica Britannica from 1950 to 1965. His book, The Interpretation of Music (London, 1954), was highly influential; he also wrote numerous seminal articles on aspects of musical sources, performance and interpretation.
In the 1950s he participated in annual concerts featuring four harpsichordists, the three others being George Malcolm, Denis Vaughan and Eileen Joyce. In 1957 this group also recorded two of Vivaldi's Concertos for Four Harpsichords, one in a Bach arrangement, with the Pro Arte Orchestra under Boris Ord. They also recorded Malcolm's Variations on a Theme of Mozart.
Dart's distinguished students included the composer Michael Nyman, conductor Sir John Eliot Gardiner and conductor/musicologist Christopher Hogwood.
He made one of the first historically informed recordings of the Brandenburg Concertos with the Philomusica of London. He later worked with Neville Marriner on a recording of both the Brandenburg Concerti and the four Orchestral suites though Dart died before this was complete.