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He and Glen Rebka first observed the gravitational redshift of light in a terrestrial laboratory. He was also involved in the discovery of nuclear magnetic resonance. Amazingly, although he was on the Harvard faculty for many years and even served as physics department chairman, he never earned a Ph.D.!
http://www.nytimes.com/2010/04/20/us/20pound.html
http://www.nytimes.com/2010/04/20/us/20pound.html