Here be the things I enjoy! Forced domesticity (because you can stand sharing the same apartment or room with guy/girl until you finally give in), hurt/comfort, blowing off steam... and yeah I looove firts time fics. I had them meet prior to SHIELD and Natasha's recruitment in one of my fics (the one I should finish), and they spent a night together for pure fun. They connected too, and it was based on "I like this other human being, I choose to do this with him/her, I am enjoying this and myself and other person". Now they've met again, in different circumstances and I think it's a matter of moment when they'll reach for each other again - for connection, comfort, blowing off the steam, name it. And then I have entire series about growing intimacy through sexual encounters. And just lots of fics where they do it, for one reason or another.
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This calls for a ficlet! *ponders*