That is some good stuff. I think the limit mentioned in the paper is related to a grain size below which the Hall - Petch relationship does not work in terms of predicting strength changes based on changes in grain size. 20 nm is very fine. The finest I've heard of in knife steels in from friction forged D2, and is about 1/4 the diameter of ASTM size 14 or 15, but even that isn't down to 20 nm.
The theoretical limit I heard was larger than what Grange was able to do. That's why I was trying to find the reference so I could maybe see the theory behind the limit. As far as I can tell, grain size is only limited by the amount of control one has over the processing. The DOE paper does interestingly mention a possible point where not only are there no more gains in properties, but they actually reverse themselves and start getting worse, ie lower strength, lower hardness, lower toughness, lower fatigue limit, etc. Heaven knows how small one has to go before that happens, if it happens in the particular material.