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Jefferson's TheodoliteMonticello houses the premier collection for the comprehensive study of Thomas Jefferson. The estate's main house, its dependencies (such as a kitchen, cook's room, wine cellar, etc.), Mulberry Row (site of light industry and slave dwellings), the surrounding gardens and grounds, and the greater plantation are the Foundation's most precious artifacts. Ongoing, systematic preservation efforts are evidence of the Foundation's long-term commitment to the preservation and restoration of the house and its authentic landscape. Monticello's curatorial collection currently includes approximately 5,147 artifacts, books, and works of art connected to Jefferson and the Monticello community. Artifacts relate to virtually every aspect of Jefferson's diverse interests in natural science, literature, history, art, Native Americans, books, works of art (paintings, drawings, sculpture, engravings), decorative arts (furniture, textiles, silver, porcelain, clocks), scientific instruments, and personal items and memorabilia such as clothing, pistols, jewelry, sewing scissors, etc. About 75 percent of these collections are exhibited; the remainder is available for study. Jefferson originally owned 60 percent of the artifacts on display.

Jefferson copy of Virgil's AeneidWithin the collection are several of Jefferson's own books among about 1,900 books with titles and editions acquired to duplicate Jefferson's original library. In addition, the collection contains over 300 pieces of furniture acquired by Jefferson in Williamsburg, Philadelphia, New York, London, and Paris, or made by Monticello slaves in Monticello's own joinery or woodworking shop; scientific instruments, such as telescopes, theodolites, botanic microscopes; approximately 500 household accessories, including French, English, and Chinese ceramics, and French, English, and American silver; and 500 works of art, including sculptures (chiefly portraits of men admired by Jefferson - Washington, Lafayette, Franklin, etc.), engravings and paintings, and portraits of Jefferson himself (including the 1805 "Edgehill" portrait of Jefferson by Gilbert Stuart, which is co-owned with the National Portrait Gallery).

Recent acquisitions include scientific instruments such as an orrery and solar microscope; a pocket globe; engravings; books; high-quality painted reproductions of original portraits owned by Jefferson (the famous Joseph Wright portrait of George Washington, Joseph Boze's portrait of Lafayette, Mather Brown's portraits of John Adams and Thomas Jefferson, and Isaac Newton and Francis Bacon from the Royal Society, London); a filing press and Campeachy chair made by African-American slaves in Monticello's joinery; books, silver, and a chair belonging to Jefferson; engravings; and John Binn's Declaration of Independence. The terra cotta patinated bust of Jefferson done from life by Jean Antoine Houdon, previously on loan to Monticello, was given to the Foundation in December 2001 by The Gilder Lehrman Collection.