Gnarls Barkley’s kaleidoscopic soul-funk thrills are also some of pop music’s most gut-wrenching deep dives into the psyche. Just listen to the duo’s massive 2006 debut hit, “Crazy,” an infectious slice of neo-soul injected with producer Danger Mouse’s bass-heavy, Spaghetti Western-flavored minimalism and powered by singer/songwriter CeeLo Green’s booming bellow. “I remember when I lost my mind,” he howls, “there was something so pleasant about that place.” The song beautifully blends pop’s sleek simplicity with soul’s raw emotion, and it was the perfect introduction to one of the decade’s most eclectic pairings. Danger Mouse (born Brian Burton) first met Goodie Mob member Green (born Thomas DeCarlo Callaway) in the late ‘90s in Georgia. Their first collaboration came several years later, when Green appeared on a 2004 bonus track off Danger Mouse and Jemini’s hip-hop album Ghetto Pop Life. By the time the pair officially became Gnarls Barkley in 2003, they had created quite a buzz—especially Danger Mouse, who had pulled off a stunning Jay-Z/Beatles mash-up with The Grey Album and produced Gorillaz’s 2005 album Demon Days. Buoyed by “Crazy”—which won a Grammy for Best Urban/Alternative Performance—their 2006 debut, St. Elsewhere, teems with giddy hooks, spliced-up beats, psychedelic riffs, a Violent Femmes cover, and crate-digging samples from Italian composers and obscure folk artists. Green’s rich voice devilishly cuts through it all, turning dark ruminations into surrealistic fantasies. The duo returned with 2008’s The Odd Couple, streamlining their brooding retro-futurism into slinky grooves like “Who’s Gonna Save My Soul” and leaving us—still—anxiously salivating for more.