Steel is a crazy world and metallurgy is a field all in itself(a field I do NOT major in, but one that fascinates me). As you're aware, "hardness", "tensile strength" and "toughness" are not the same things. Hardness may well improve resistance to wear but it will not improve structural integrity. In fact, for a given alloy, as hardness increases, toughness decreases. Now nitrating or similar processes only affect the exposed surface (much like case hardening) and therefore leave the substrate material alone(ie tough). But if you're after a superior material, then that is what you have to start with.
As my boss used to say, "4140 is pretty darn good stuff". And it is. with a tensile strength of 98-125k psi depending on condition it is a standard by which many steels are compared.
17-4 stainless is awesome stuff. Depending on the condition, it can have similar tensile strengths to 4140 and is orders of magnitude superior to 416ss with its(416's) tensile strength of 75-85k psi.
4340 is mucher heavier dutier stuff, having a tensile strength of up to 165k psi. Generally we use this when 4140 wont quite do the trick.
There are many many other options out there of course, but these are a sampling of commonly referenced alloys.
If you aren't able to find Lothar Walther blanks or another "off the shelf" solution, I will soon be able to make barrels out of pretty well any alloy you wish. My rifling machine is 90% finished (my electrician is currently wiring it up and I hope to be able to start motion testing in the next week or so). I may sound forward/arrogant, but I'm honestly not someone to make claims I can't make good on. If you want something built that is out of the norm, I am very confident I could help make it happen.
Your project is one that interests me, I'd be willing to make a few test barrels with you and see how thin/hot they can be pushed before failure... feel free to shoot me a pm if you're interested.
Regards,
Paul.