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There is no such thing as 'most important gas' regarding weather.

Weather is affected mainly by temperatures. Temperature is affected by geology. The greenhouse effect is fundamental in affecting global temperature.

Thus carbon dioxide and water vapour are very important. The ecosystem is fundamental in affecting gas concentrations. The explosion of life in the oceans resulted in the decrease of carbon dioxide and corresponding increase in oxygen in the atmosphere. Nitrogen is essential for life and atmospheric nitrogen is thus also very important.

Basically, all gases are very important to weather process, but not necessarily directly.

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