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According to most artists, the large eyes are supposed to signify the supposed innocence of the characters in their early years of life. Now take into consideration that young in anime is anyone under 30, or is that 3000 for some of the more out there series.
For a stark contrast to the phenomenon, watch Ghost in the Shell. All characters are intended to be further in age and certainly not innocent in any way imaginable, thus the facial animation is more true to life as expected. Only at the end of the first movie does the large eyes play into the scenes, as Motoko is transfer to the body of a young girl.
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Watching a little too much hentai lately?