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The only photo of her that shows this eyes-wide-open look is the one at the top left and it's definitely a deer-in-the-headlights look.
In the other photos her eyes look more relaxed and natural. In those photos the amount of the top half of the iris that can be seen is much less.
To a lesser extent, the staring look she has in the painting (in the eye on our left, particularly) is due to the sharpness of all those eye edges and the extreme contrast between the iris and the white of her eye.
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