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Andrea,
Whenever I talk a client out of a "laughing face portrait" I feel as if I've dodged a bullet. I have a terrible time trying to make them look "natural". You might wander through the SOG stable of artists to see if you can find someone who paints them well, and study what lighting he/she uses. The strong outdoor light you have in your portrait also is making it hard for you to find attractive shadow patterns. Good lighting is EVERYTHING in portraiture.
You might also explain to your client that a photo is different from a painting on many levels and that an expression that is perfect for a photo may not be successful in a painting. Clearly this is a lively, happy child and you can show her happiness in other ways than a flat-out laugh.
I agree with Michele - take as many more photos as you need and take your time with the head.
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