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Of the ones you posted I like #3 the best, but as Chris mentioned, there's a problem in all of them about the light direction. The boy's face has light coming from two directions and the girl's face has just one, for example.
I also wouldn't choose a composition where one of the heads was much larger than the other, even if it's because one kid was closer to the camera. It sends a message about importance that you and the parents may not want. The key to solving that problem is during the photo shoot -- the camera should not be too close to the subjects and then any difference in sizes due to distance will be minimized.
Also, how do you plan to handle the girl's braces? Paint them as they are? I've painted a couple of kids with braces and we go for a closed-mouth smile on those portraits.
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