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He made major contributions to the theory of approximate molecular orbital (MO) calculations, starting with one identical to the one developed by Rudolph Pariser and Robert G. Parr on pi electron systems, and now called the Pariser-Parr-Pople method.
Working with DuPont chemist Rudolph Pariser, Parr developed a method of computing approximate molecular orbitals for pi electron systems, published in 1953.