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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.

The contents of the collection include: correspondence, manuscripts, minutes of "Zagranichnai︠a︡ Delegat︠s︡i︠a︡" meetings from the 1920s, and financial records both from the Party organization in Russia (1908-1915) and from its Estonian and Finnish affiliates (1922). The collection's subject files are particularly rich in materials on S.R. groups in foreign countries and on Party infiltrators ("provokatory"), including E.F. Azef. The collection also contains photographs of several prominent S.R.s, including Ekaterina Breshko-Breshkovskai︠a︡; printed materials, including the first five issues of "Sot︠s︡ialist Revoli︠u︡t︠s︡ioner (1927-1932); and seals from the offices of the "Zagranichnai︠a︡ Delegat︠s︡i︠a︡." Correspondents which figure prominently in the collection are: Nikolaĭ D. Avksentév, Viktor M. Chernov, Ili︠́a︡ I. Fondaminskiĭ, Osip S. Minor and Vladimir M. Zenzinov; there is one letter by Azef. Much of the pre-1920 correspondence is addressed to Mark A. Natanson; after 1922 a large number of the letters are addressed to Sergeĭ P. Rostnikov.