Fundamental to the question is displacement of the take (total physical volume). Once you get to a tank that is neutral when empty, it weighs the same as the water it displaces... any lighter and you need lead to offset the positive buoyancy. In order to make that work in your favor, you need higher pressures to get the same volume of air in a smaller space (less water displaced) otherwise it's a zero sum game. Most regs are designed to for 3000-3500 psi tanks, get much over that and you increase wear rate and likelihood of HP seat failure. So, to answer your hypothetical "what would it take" to include unobtainium materials, aim for a 10k psi tank 1/3rd the size of an Aluminum 80. If your unobtainium is can achieve those pressures at 10 lb total weight, it would be neutral when empty. And bankrupt a small nation to produce. That's where Lex's comment on old school 72's comes in. They weigh about 26 lb, and are neutral empty.... overfilled to 3000 psi they are 85 CF. I have 5 and am always keeping my out for more on the cheap!
Respectfully,
James