Do they pop out of gear in all selections? or is it just a 4hi or 4lo thing?
One thing I had planned down the line was 4:1 gears and some sort of under drive setup in front of it. Northwest fab just came out with a new one that adds only 5" to the overall length. It should crawl great after that 
NOW, on to the results of my visit to TLC Transmission. Driving the jeep did not yield any noises (must have scared them away) but once on the lift, the "chatter" (it sounded more like a rattle outside of the jeep) was easily recreated. Lee crawled under the Jeep with a stethoscope and believes the noise coming from the transfer case (it was loudest there), although he also said there was some noise coming from the transmission. Thanks again for the help Lee.