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While his output diminished after Surrealistic Pillow (1967) as Slick, rhythm guitarist/singer Paul Kantner, and lead guitarist Jorma Kaukonen matured as songwriters (a process compounded by Balin's eschewal of the group's burgeoning "ego trips"), his most enduring songwriting contributions—which were often imbued with a romantic, pop-oriented lilt that was atypical of the band's characteristic forays into psychedelic rock—include "Comin' Back to Me" (a folk rock ballad later covered by Ritchie Havens and Rickie Lee Jones), "Today" (a collaboration with Kantner initially written on spec for Tony Bennett that was prominently covered by Tom Scott), and again with Kantner, the topical 1969 top-100 hit "Volunteers. " Although uncharacteristic of his oeuvre, the uptempo "3/5 of a Mile in 10 Seconds" and "Plastic Fantastic Lover" (both written for Surrealistic Pillow) remained integral components of the Airplane's live set throughout the late 1960s.

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