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Lighting is a very involved subject and I don't have the time to go in great detail but here's the gist of what I see:
The little girl's photo has the light coming from the lower right and the side. Lower sourced lighting looks unnatural because in the natural world the light comes from above. They use this kind of lighting in horror movies, but in a much more exaggerated way. Also, the mouth being open is not appealing.
The little boy's lighting is more from the side. Side lighting can work but not so well when you are looking into the shadow side. Side lighting, the way you have it exaggerates the thinness and pointedness of the face.
Lighting for painting is different than lighting for a photo. Photos are more acceptable because we've come to trust that what the camera sees is real. In a painting all bets are off. I know this is an over simplification but the front of the head should be lit to emphasize the form, with at least 3/4 of the face in light. This rule can be broken but should be for a specific reason. Check out old master portraits and see what they did.
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