Problem with surfaces vs volumes

I'm not sure what you refer to... The NxN coherence with the options configured as mentioned before, you should obtain one value per pair of scouts. Try with simply two scouts to understand what is going on.
If you think you are not getting what you should, please post a screen capture where you see this "3x90" values.

Indeed, the atlas of deep structures use only fully unconstrained source models.
See this tutorial for more information: http://neuroimage.usc.edu/brainstorm/Tutorials/DeepAtlas

I don't know what Cartool does or not, you'd have to ask Denis Brunet.