In 1968, Jarreau made jazz his primary occupation. In 1969, Jarreau and Martinez headed south, where Jarreau appeared in such Los Angeles hot spots as Dino's, The Troubadour, and Bitter End West. Television exposure came from Johnny Carson, Mike Douglas, Merv Griffin, Dinah Shore, and David Frost. He expanded his nightclub appearances performing at The Improv between the acts of such rising-star comics as Bette Midler, Jimmie Walker, and John Belushi.

In 1975, Jarreau was working with pianist Tom Canning when he was spotted by Warner Bros. Records and soon thereafter released his critically acclaimed debut album, We Got By, which catapulted him to international fame and garnered him a German Grammy Award. A second German Grammy would follow with the release of his second album, Glow.

One of Jarreau's most commercially successful albums is Breakin' Away (1981), which includes the hit song "We're In This Love Together." He wrote and performed the Grammy-nominated theme to the 1980s American television show Moonlighting.

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