Physical Chemistry underwent a transformation from a science based on thermodynamics to one based on quantum mechanics in the 1920s and the early 1930s. Although quantum mechanics was born in Germany and first applied to a chemical problem, understanding of the covalent bonding in H2, by two physicists, Walter Heitler and Fritz London1, the transformation in physical chemistry was mainly made in the US; some young American physical chemists were very active in applying quantum mechanics to chemical problems. Most notable among them were three Nobel Prize winning physical chemists, Linus Pauling, Robert Mulliken and Harold Urey. In particular, Linus Pauling and Robert Mulliken played the most important roles in the development of quantum chemistry in the 1920s and the1930s. Both of them started as experimental physical chemists, Pauling as an X-ray crystallographer and Mulliken as a molecular spectroscopist, but they became pioneers in applying quantum mechanics to chemical problems. However, in their endeavors they took different approaches. Pauling advanced valence bond theory, applying it to explain a variety of chemical bonds. His famous book on the nature of chemical bonds was well received by chemists and became a classic.2 On the other hand, Mulliken advanced molecular orbital theory in connection with the interpretation of the electronic spectra of small molecules3. Before World War II Paulings’s valence bond theory was more popular and influential among chemists because of its appeal to chemical intuition. However, in the long run Mulliken’s molecular orbital theory has made a much greater influence on chemistry as performance of electronic computer improved rapidly, while Pauling’s valence bond theory eclipsed. Among quantum chemists Mulliken made the most important contributions to the transformation of chemistry in the period covering from the 1920s to the 1960s. He also presented a theory on charge transfer (CT) complexes in 1952 that has become very influential in a variety of areas of chemistry.4 This theory made a particularly strong impact on Japanese Physical Chemistry.
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