I'm well aware of that. I grew up on Batman too, who is of course the King of Brood. I'm not saying DB is the Best Brooder Ever, or that Angel is the best written incarnation of that archetype, just that he gives a better performance than he's often given credit for. However, I don't have an extensive knowledge of how that archetype has been used throughout film and TV history so I couldn't possibly thoroughly evaluate where he rates on the scale (seriously - not being sarky here.)
I'm not sure the odd gif does much to support your argument because unless you're willing to upload dozens of them, it's difficult to properly convey the emotional fluctuations a character goes through over one episode or even one or two scenes. As it is I don't see any brood from that
Punisher shot, more like blank staring (but like I said, difficult to judge the character based on a single gif). And in the one of Angel below that I don't think he
is actually brooding in that scene. It's not his brood-face, which goes more like this:
(sorry for the giant image. Couldn't find a smaller one)
He seems to be responding to another character but I can't tell what episode that shot is from. So not the best example.