This is a fairly understated scene, but I think his quivering lip is really charming.  

http://video.anyclip.com/movies/control/deep-depression-and-another-seizure/

I recommend the whole film, especially for anyone who is interested in Joy Division -- it's an excellent biopic of the band's lead singer Ian Curtis.  The black and white cinematography is stunning.

I know the film features more intense crying scenes from Riley -- as this GIF attests:



And also -- I'm fairly sure -- from Samantha Morton who plays his wife.