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The series is arranged in three sub-series: general correspondence of Eugen Spiro, 1903-1913 and 1941-1972; correspondence with owners and subjects of Spiro paintings; and correspondence of Lilly Spiro, primarily dating from the years after Eugen's death, 1972-1985. Among the noteworthy correspondents are: Tilla Durieux, Albert Einstein, George Grosz, Theodor Heuss, Otto Loewi, Thomas Mann, Dimitri Mitropoulos, Albert Schweitzer and Gottfried Reinhard Treviranus.

German-Jewish painter interned in the French concentration camp at Gurs, painted portraits of Thomas Mann, Albert Einstein, and other notables. The collection includes correspondence, photographs of Spiro's artwork, and exhibit catalogues.