Little Good Omens Headcanon of mine:
We know that Gabriel's eyes are a vibrant purple in Good Omens. Some theorize thay his eyes are purple because he's supposed to represent the most beautiful man, and the most beautiful woman, Elizabeth Taylor, also had violet eyes. Others theorize it has to do with being the Supreme Archangel of heaven.
I think it's both to a degree.
See, I theorize that Gabriel thinks very highly of himself, maybe even to a narcissistic degree. We can see that as he admires the statue of himself in the cemetery. He saw himself in someone who was valued as "the most beautiful," and so when he was appointed as Supreme Archangel, his status manifested in the color purple. Purple eyes and a purple accent color (his tie). It reflects a form of love or an angel equivalent.
I've seen people draw Supreme Archangel Aziraphale with purple eyes, and while I think that looks cool, I don't think that's what his eyes would look like.
In Season 2 episode 3, Aziraphale is driving Crowley's Bentley, and we see that it's yellow. He finds fondness and comfort in the color. And the Bentley doesn't mind either, considering it was content with Aziraphale and his driving style and preferences.
Now, what else is yellow in the show?
And when do we see Crowley's eyes the most?
With Aziraphale in his bookshop, the only place the demon feels comfortable to expose his eyes when in the presence of others.
So my theory is that when Aziraphale is officially appointed as the new Supreme Archangel, his eyes will shine yellow, the same yellow as Crowley's eyes. He'll probably have an accessory that is also yellow (tie, scarf, something) like Gabriel did with his tie. It will not only show his new elevated status but his devotion and still cherished love of Crowley even if they're on terrible terms at this point.
Imagine how off-putting that would be to the other angels, too. Here is this heathen, this human lover, this demon conspirator, now appointed to the highest position an angel, and his eyes are just like of the fallen one. The demon he's spent so much time with has obviously imprinted on Aziraphale in such a capacity that, even though he chose Heaven, the demon is still with him. He's been influenced so deeply that it reflects in his angelic nature.
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