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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".

While employed at Arthur D. Little, Dr. Vonnegut built upon his research in atmospheric science. The majority of his work focused on electrification of clouds, thunderstorms, and the behavior of lightning, he also looked at behaviors of gases but on a much smaller scale. Besides pursuing his own research, Dr. Vonnegut worked on a number of advisory projects for the United States government. These projects focused on the relationship between aircrafts and lightning. The main focus was on how aircrafts detect and avoid lightning when flying in a storm.

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.