From the pics, it looks like some competent work was done. No shade-tree stuff going on that I can see. Also the elimination of the axle ratios and hubs was good news. Soooo....
The only thing I saw was in one of the photobucket pics. The shot of the front of the truck shows what looks like the front tires toed-out pretty far. Not sure if the truck was still under construction at this point, but the tires should be aligned to be toed in 1/16-1/8". Never out. That could cause wandering.
As far as the caster, 4.5 deg is good as long as that's the absolute measurement (with the truck on a level pad at normal load) and not a number the shop added, and is quoting now.
If you could drive the truck onto an alignment rack and see 4.5 deg positive, you're fine.
As far as the grinding going into 4wd, we've eliminated the obvious things. Not sure where to go from here. When its in 4wd, you say you have major shaking. If your axle ratios were different, you'd really not be able to move it very far before it bucked and bounced you out of the chair. But if its a vibration, and happens above say 25 mph, then that could be your front drive shaft. It doesn't have the cv joint at the top, so you do have quite a bit of angular imbalance. Check this video. Makes it plain as day. Is this what you're experiencing?
https://www.youtube.com/watch?v=gmv4qwlfomy
I don't see how fixing the front drive shaft will cure the 4wd shifting issue, but its possible that your shaking in 4wd will go away.
Another thing is to check the phasing of the front drive shaft. Both yokes need to be on the spline parallel as you look at it from one end. If its off one spline, there would be vibration.
If it were me, I'd look at the toe adjustment. If its good (hard to tell from the pic), take it for a spin in 2wd, hubs unlocked. If it still wanders unacceptably, then you'll have to have someone confirm the caster and toe settings. If it goes down the road ok, then how's the vibration? If its ok, then lock in the hubs and try it again. Hubs locked in 2wd will spin the front drive line and probably give a vibration. Should be more of a buzz and not as destructive as it seemed in 4wd.
If it still bucks and jumps around in 4wd, all I can say is put it up on blocks and verify the front tires spin at the same speed as the rears. Tires are the same size front and rear, right? That would also cause a slight ratio mis-match. Other than that, I'd say you still have a gear ratio that's different in one axle.
Maybe one of the real braniacs will chime in and pour some fresh science on this fire....I think I've covered all of the possibilities I've run across.
Let us know...
Just seeing your reply. I was a little late and didn't see it.
Sounds like you're on the right track now....!