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The materials that comprise the Vertical File have been collected and added to from a variety of sources by former Avery Librarians. The vertical file contains clippings, pamphlets, reprints, and other miscellaneous materials relating to persons, places, organizations, and topical subjects relating to architecture, housing, and city planning. The purpose of the vertical file was to arrange and store small items, memorabilia, and ephemeral material on a variety of topics to facilitate access by researchers. For the most part, the vertical file contains printed items only. Manuscript material and other unique items were, generally, not placed in the vertical file. In some cases, manuscript material has been removed from the Vertical File and placed in its corresponding collection.

The bulk of this collection consists of more than 22,000 black and white photographic negatives and more than 10,600 black and white photographic prints documenting commercial, institutional, religious, and residential architecture throughout the United States, with particular emphasis on sites in the mid-Atlantic region. These images date from the mid-1930s to Molitor's retirement in the mid-1980s, with the great majority of images created between 1946 and 1980. Also included in the collection are images of landscapes, industrial design, portraits, and events of personal significance to Molitor. In some select cases, color prints, color negatives, color transparencies, and 35mm slides are also available in addition to or instead of the black and white negatives and prints. Researchers are also advised that documents in this collection indicate that when faced with a lack of storage space in 1973, Molitor contacted clients to return inactive negatives that they had comissioned before 1955. In at least some cases, those clients declined to accept their negatives and Molitor subsequently destroyed the images. Thus, this collection has lacunae in the negatives series.