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This series documents the Project Cirrus program, a weather modification initiative undertaken by GE along with the United States Signal Corps, Office of Naval Research, and the United States Air Force, with general oversight handled by the Department of Defense. As part of the effort, Dr. Vonnegut discovered that AgI, Silver Iodide, was a superior nucleation agent. This discovery significantly influenced the science of artificial precipitation and this method came to be adopted as the chief means of "rain making".

Series 4 documents Dr. Vonnegut's work with the New Mexico Institute of Mining and Technology (NMIMT) in Socorro, New Mexico. While both were employed at Arthur D. Little, he and fellow scientist Charles Moore were invited to conduct thunderstorm research at Mt. Withington, eventually becoming part of the Langmuir Laboratory for Atmospheric Research in Socorro. Moore stayed at NMIMT, and Dr. Vonnegut moved on to the State University of New York at Albany; though their collaborative research continued for the entirety of each other's career.

This series consists primarily of tornado observations and eyewitness accounts solicited from the general public via newspaper advertisements in areas where tornadoes and severe storms frequently occur. They are filed using the original labeling system employed by Dr. Vonnegut, where the date and place of the observation as well as a brief statement on the phenomena is used to identify the observation. Accounts of severe storms found in multiple publications, biblical references, and other historical observations are also present.