Are you talking a choice between 2GB 680s or a 4GB 690 (which is still only 2GB usable memory)?
If you're running surround, I assuming you mean 3x1080p screens, you're going to run out of VRAM I think. Do they have a 4GB option on the 680s, or anthing from the 7xx serious or an AMD equivalent (high end AMD cards tend to scale better at higher resolutions)?