He then moved to the University of Maryland, where he became chair of the Department of Physics and Astronomy in 1953. During his tenure as chair, he was responsible for a major increase in size and quality of the department. The physics building at the University of Maryland is named for him.
In 1965 he left to become the second president of the State University of New York at Stony Brook, a position he held until 1978. While he was there, Stony Brook University, one of four SUNY centers created by then-governor Nelson Rockefeller (briefly Vice President of the United States under Gerald Ford), and, until recently, the only four allowed to call themselves "universities", grew to more than 17,000 students from a handful who started their academic careers before the campus was even finished, at the now-defunct State University of New York on Long Island (SUCOLI).
In 1995, at age 71, he became president of Washington College, a small, private liberal arts school in Chestertown, Maryland. There, he was credited with fixing the school's budget crisis and raising its national profile.
He married the former Deborah Taintor, and they had two daughters. Toll died on July 15, 2011, of respiratory failure at Fox Hill Assisted Living in Bethesda, Maryland.[4][5][6]