HRS (hot rolled) should be preferred as it's more or less in annealed condition; CRS's internal stresses will trap magnetic fields (again, in most steels, metallurgical "hard" is also magnetically "hard", as far as I know).
Mill surface won't be very flat though. You'll presumably need to machine something, either way, so that shouldn't be a problem, but it hasn't been mentioned if you have that capability?
Yeah, flux return is great, look at the classic pictures of, well, circlotrons for example, as our fellow forum member so kindly
is -- often a boxy figure-eight shape, steel looping around the outside, with an electromagnet on the middle limb (you'd stack your magnet(s) here), and the pole pieces and gap on it as well.
Welding shouldn't be too much of a problem, by the way; even less so if you have the capability to anneal the assembly once finished. That'll also relieve internal stress, which will definitely be present after welding.
I don't know how much this kind of on-the-fly redesign matters to a magnet; I would think, if you have the means to probe its homogeneity, and the ability to shim accordingly, you should be able to do so for any reasonably similar design. The significance of, for example, the flux return, should be of more than doubling the flux density in the gap, which is definitely a worthwhile gain!
Magnets I think, tend to be discouraged because of their drift and tempco? I know the original experiments (Purcell, et al.) were done with electromagnets ran from lead acid batteries (and, no lie, thermally regulated via grad-student-controlled windows), but we probably don't have to go quite to such lengths nowadays. A nice strong water reference and some kind of tracking PLL may be good enough instead?
In any case, will be interesting to see if you get any detail out of this; not sure if chemical structure (frequency shifts of ~ppm) will be resolvable at these field strengths, or with reasonable acquisition times (or at all), but if so, that'll be freaking awesome.
Tim