That is a huge shim. You may need 2-3 degrees in there, but that looks like 10 or more to me. Just measure it with an angle finder and then do the simple math. Much easier than doing it over and over again. When you take out the shim (and any leafs) the angle at the T-case output will get a little smaller. Aim the pinion like 2 degrees lower than where the T-case output angle is now.
The BEST way to put in shims and blocks is to run the center-bolt down through the whole stack - leafs, block, shim, etc. This makes the whole thing like one big spring pack and is much safer than having a hole and a nub on the block. You can usually score new center-pin bolts at big-rig or driveline shops for a couple bucks. The reason it's hard is that the top of the bolt and bottom of the bolt rest on different angled surfaces. They make tapered shims that go under the head of the center-bolt to solve this. The taper should match the taper of the shim.
It looks like your U-bolts are brand new and they should come right off.