Well this isn't as specific as you asked for, but I'd like to say Yokushitsu/La Salle de bain. Between these two incarnations of the same song, I can feel almost everything that SR represents for me. It sounds both rough and polished at the same time. With La salle you get her "disney" sound, but Yokushitsu gives you the SS edge. It's both experimental and accessible. You can hear it and say "This sounds crazy as hell but I want to hear it again", and that goes for both versions. So it's not exactly a moment, but this song totally explains why I love Shiina Ringo.
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I was floating on a breeze
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