I think there might have been a serious/flashback episode like Hiro's before - the Natsume origins episode. So much of the show's more dramatic material (and just as much of its fluffy softness) revolves around this trio. Yuno's meeting with Arisawa back in ☆☆☆ also comes to mind. While it's not ground the show treads very often, when it does, it handles it well.
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