Put it at the peak of a scare or fail, right before the reaction shot, then follow it with the Oh My God Meme for disbelief and the Scream Meme for a second reaction. Keep it as the first reaction, so the later sounds build on it instead of repeating it.
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This is a very short, high-pitched Luigi scream lasting under a second, a sudden cartoon yelp delivered in a strained, panicked voice. It feels frantic and funny, the kind of over-the-top reaction that turns a small scare into a joke. The burst is too quick to build up, so it lands as pure surprise.