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About title chance, are you sure No rises significantly if Barca doesn't win? I need to really spend some time here one day because I feel like I'm missing out

I can’t give you a straightforward answer, because, as you rightly noted, what we have here isn’t roulette - it’s a combination of mathematical side and the opinion of the crowd.
In terms of the purely mathematical side of things, we are now heading into the 12th round out of 38, and it’s blindingly obvious that no single outcome should significantly shift the range of possibilities.
I'm looking forward to a potential shift in crowd opinion. For starters, I believe the current odds are distorted, while Barcelona is playing with flair and conviction, that in no way justifies the notion that they have a 68% chance of securing the title - especially with two challengers close behind, where a single poor performance could see Barcelona drop all the way to third place. In other words, the first factor is that there is room for price movements within the existing figures.
What happens if Atlético wins? Looking at the math: how can they have a 68% chance of winning the title if, for crying out loud, they’re dropping to third place? What will the public sentiment be like if Atlético wins? It seems to me that everyone would then realize that three defeats in three major matches is a bad sign, and Barcelona would no longer be so overvalued - meaning the implied probabilities would shift from 68% down to, say, 55-60%. For the "No" outcome, this would be equivalent to a move from 33% to 40-45%, which translates to profit of 21%-36% (for my bet on No).
On one hand, it’s not much, on the other, it’s perfectly normal - even if Barcelona were to win 10-0, the crowd's spirits won't rise much higher, as they are already in the heavens which means the bet on "No" won't lose much of its value.
In terms of emotional stakes, the upcoming match falls into one of two categories: either a massive disappointment for Barcelona, or a "things going exactly as expected" scenario. I see a significant imbalance in this assessment, which creates an opportunity to profit. Given that Barcelona is highly likely to win, we’ll be able to see in practice just how much their odds, currently sitting at a 68% implied probability, actually shift. I would be very surprised if they surged significantly, rather than just nudging up by a couple of percentage points.