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The collection consists of correspondence, manuscripts, notes, photographs, subject files, and printed materials. Correspondents include Victor Chernov and George Kennan. Extensive notes by Mosely concern European diplomacy in the 1830s and the South Slavic Zadruga. There are thousands of photographs, chiefly from the Soviet Union ca. 1945-1955. Besides photographs of Soviet, Chinese, and East European political figures, such as Mao Tse-Tung, György Lukʹacs, and Boris Spasskiĭ, there are photographs of such Western figures as Enrico Berlinguer and Pablo Neruda. Subject files and mimeographed and printed materials include files on the Inter-University Committee on Travel Grants; papers on Soviet Studies distributed by St. Antony College, Oxford University; State Department research reports, and works by Mosely.

Correspondence, manuscripts, and subject files on most aspects of Pegram's career. Also, a large quantity of research notes made by Lucy J. Hayner (1898-1971), Professor Emeritus of Physics at Columbia University, who was writing a history of Columbia's Physics Dept., 1905-1954, can be found in folders throughout the collection.