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The terms atom and molecule were used interchangeably until the early 19th cent. Initial experimental work with gases led to what is essentially the modern distinction. J. A. C. Charles and R. Boyle had shown that all gases exhibit the same relationship between a change in temperature or pressure and the corresponding change in volume. J. L. Gay-Lussac had shown that gases always combine in simple whole-number volume proportions and had rediscovered the earlier findings of Charles, which had not been published.
Dalton's Theory
One early theorist was John Dalton, best known for his atomic theory. Dalton believed that gases were made up of tiny particles, which he thought were atoms. He thought that these atoms were stationary and in contact with one another and that heat was a material substance, called caloric, that was contained in shells around the atom (these shells of caloric were actually what was in contact). When a gas was heated, the amount of caloric was increased, the shells became larger, and the gas expanded. Dalton d's findings about combining volumes of gases, perhaps because it could not be explained by his theory.
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