What light gas can I have in the upper atmosphere?

I want to have an upper atmosphere composed of a gas which is lighter than "air" so that my human occupants of a planet can harvest it and use it to fill blimps and hot air balloons.

I'm planning on having my "normal air" as Nitrogen Oxygen as I see no need to change it from Earth-like. I'd rather not use have a Hydrogen layer (as it explodes and would ignite both balloon and planet).

Is it possible to have a layer of Helium in a planet's upper atmosphere (which then the humans could use some dodgy hydrogen balloons to reach and harvest).

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What light gas can I have in the upper atmosphere?

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