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Following the resolution of the war, Leary decided to pursue an academic career. He described himself during this period as "an anonymous institutional employee who drove to work each morning in a long line of commuter cars and drove home each night and drank martinis ...
To the chagrin of his family, Leary elected to transfer to the University of Alabama in late 1941 because of the institution's expeditious response to his application.
In addition to his teaching duties, Leary was affiliated with the Harvard Center for Research in Personality under Mc Clelland and oversaw the Harvard Psilocybin Project and concomitant experiments in conjunction with assistant professor Richard Alpert.