As long as you avoid condensation, the cold won't hurt your CPU. However, you may find that for your purposes, all sub-ambient cooling methods are beyond the point of diminishing returns. If you haven't tried ambient watercooling yet, I suggest you start there. If you decide later that the slight increase in performance is worth the increased complexity and power consumption of a phase change system, the experience you gained with your ambient rig will be very useful. Odds are good, though, that ambient watercooling will be enough.
OTOH, if you're refrigeration tech with too much time on your hands and just want to mess around, you'll find plenty of good ideas in the extreme cooling section.