In his analyses of air Dalton made use of the old nitric oxide method. In 1802 this led to an interesting discovery. If in a tube .3 of an inch wide he mixed 100 parts of common air with 36 parts of nitric oxide, the oxygen of the air combined with the nitric oxide, and a residue of 79 parts of atmospheric nitrogen remained. And if he mixed 100 parts of common air with 72 of nitric oxide, but in a wide vessel over water (in which conditions the combination is more quickly effected), the oxygen of the air again combined with the nitric oxide and a residue of 79 parts of nitrogen again resulted. But in the last experiment, if less than 72 parts of nitric oxide be employed, there will be a residue of oxygen as well as nitrogen; and if more than 72, there will be a residue of nitric oxide in addition to the nitrogen. In the words of Dalton, "oxygen may combine with a certain portion of nitrous gas [as he called nitric oxide], or with twice that portion, but with no intermediate portion."
Naturally these experimental facts were to be explained in terms of the ultimate particles of which the various gases are composed. In the following year Dalton gave graphic representation to his idea of the atomic constitution of chemical elements and compounds.
( ) Hydrogen (|) Nitrogen (·) Oxygen (*) Carbon (|) (·) Nitric oxide (·) (|) (·) Nitrous oxide (·) (*) (·) Carbonic acid
Much against Dalton's will his method of indicating chemical elements and their combinations had to yield to a method introduced by the great Swedish chemist Berzelius. In 1837 Dalton wrote: "Berzelius's symbols are horrifying: a young student in chemistry might as soon learn Hebrew as make himself acquainted with them. They appear like a chaos of atoms ... and to equally perplex the adepts of science, to discourage the learner, as well as to cloud the beauty and simplicity of the Atomic Theory."
Meantime Dalton's mind had been turning to the consideration of the relative sizes and weights of the various elements entering into combination with one another. He argued that if there be not exactly the same _number_ of atoms of oxygen in a given volume of air as of nitrogen in the same volume, then the sizes of the particles of oxygen must be different from those of nitrogen. His interest in the absorption of gases by water, in the reciprocal diffusion of gases, as well as in the phenomena of chemical combination, stimulated Dalton to determine the _relative_ size and weight of the atoms of the various elements. Dalton said nothing of the _absolute_ weight of the atom. But on the assumption that when only one compound of two elements is known to exist, the molecule of the compound consists of one atom of each of these elements, he proceeded to investigate the relative weights of equal numbers of the two sorts of atoms. In 1803 he pursued this investigation with remarkable success, and taking hydrogen (the lightest gas known to him) as unity, he arrived at a statement of the relative atomic weights of oxygen, nitrogen, carbon, etc. Dalton thus introduced into the study of chemical combination a very definite idea of quantitative relationship. By him the atomic theory of the constitution of matter was made definite and applicable to all the phenomena known to chemistry.