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*Charles Coffin Jewett (1847-1855), Assistant Secretary acting as Librarian
*Jane Turner (1855-1887), first female employee of the Smithsonian, assigned as keeper of accession records for books after Jewett's dismissal
*Theodore Gill (1866 - ?), Assistant to the National Library (Library of Congress)
*John Murdoch (1887-1892), librarian
*Cyrus B. Adler (1892-1905), Assistant Secretary in Charge of Library

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