Ange is - initially - so caught up in her own little mental huffy world that she doesn't quite notice what kind of reaction her words are causing in the man.

It takes a moment or two, and then Ange properly looking back at Shiro, for her to realise what's actually going on. It seems to make the huffiness about her fade, replacing the emotion with something more akin to surprise.

"W-Wait, are you crying?"

This is some sort of ironic mirror of when she asked about him laughing a few moments ago, huh. Even the emotion behind it is entirely different. Not judging him like for the laughing, but instead--

"Shiro, you can't cry..!" P-Please! Not over her, at least?!