I think what we're seeing here is the PERS eyes having trouble reconciling itself with such an extreme facial expression. The two just don't work well together, which is why the face looks so psycho (and not Harley Quinn psycho in a good way). The eyeline isn't right either - there's too much of an upward pinch at the back of the eyes. Quinn's/Robbie's eyes have a fairly straight eyeline across her face.
For the most part, HT got it right the very first time around with the original Harley Quinn figure, back in 2016. Since then they haven't been able to capture her likeness as well. I know what it is too: they just need to fix the eyebrows and most of the face will come together. Robbie has very thick dark eyebrows, with a high arch, like you'd find with classic 40s femme-fatale vamps. If they simply add more paint and a sharper arch to the brows, everything will come together and look a lot more like the Quinn we expect to see. This is what makes Robbie so distinct and recognizable, and HT just seems to miss that glaring reality in their attempts to depict Harley Quinn in their sculpts. Look at the very first Quinn figure and you'll see how they got it mostly right that time around. Look at any others, including this "artisan" version, and you'll see how they dropped the ball.