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空{くう}気{き} and 大{たい}気{き} both share the definitions of air or atmosphere as their main definitions.

I see they both have distinct additional definitions (the former can be used for mood, and the latter for generosity), and that 空{くう}気{き} shows air ahead of atmosphere, whereas 大{たい}気{き} does the opposite (at least in Shirabe Jisho, the dictionary I'm using).

Are there specific circumstances over which one should be used over the other when referring to air/atmosphere, or are they completely interchangeable for this definition?

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空気 is normally translated as "air," the kind that you can breathe, or put into a balloon.

大気 specifically refers to the huge layer of air/gas surrounding the earth (or sometimes, another planet). You cannot breathe in 大気, nor can you put 大気 into a balloon, but you can leave the 大気 with a rocket.

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