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Is there any way to get Citrea to just stop? Like hey, 'cut it out'?
In this particular case, definitely not. Even with the "prove your bytes aren't arbitrary data" soft fork proposal they're doing something valuable enough to make grinding bytes feasible.
why don't they just use LibreRelay?
Because this type of Citrea transaction is time sensitive. Only two major mining pools mine oversized OP_Returns right now. That means there's a decent chance this type of Citrea transaction – a tx that responds to fraud – would fail to be mined.