This is knowledge I have gained through experience building my company to study these things over the last couple of years. Theres a lot LOT more to this, if youre interested I would recommend reading all the papers you can find on HEA. Getting a subscription to Advanced Materials from Wiley, and then trying to simulate some of the materials yourself. Don't start with HEAs they are hard and you need a lot of computing power, start with simple systems like bulk copper, aluminum and iron. Then move to binary systems, ternary systems and increase the complexity of what youre modelling while always checking against experimental data. Learn about all of the shortcomings of the simulations and then ask yourself "ok how can I improve that", while you're learning this you're developing an intuition for all of the settings in the simulations (whether atomistic. Meso-scale, macroscale or other)

I have a 15 GPU cluster in my house just so I can study HEAs - but I understand thats out of budget for a hobbiest so that's why I recommend you start with simpler systems and slowly increase complexity.

You might see various datasets for HEA, HEA property prediction, and synthesis predictors, but cold hard truth of the matter is that the quantum interactions at the interatomic level are so complex, the configuration space youre searching is so massive, that no dataset is going to make a dent in it, so models are only really useful as VERY VERY VERY approximate screening tools (sometimes) - and thats not even talking about micro-scale phenomena and macroscale phenomena - which are enormous subjects on their own and just as important!

You must simulate all of these, you can't just do a Microsoft Mattergen that spits out an idealized crystal structure at 0 Kelvin, because in the real world, thats barely the first step.

Seriously!

ok, so quasi-random. Would it be more useful to have such a machine to feed data back to models to better the simulations where we could do more in less time and prune down to more likely candidates?

And while you're at it, #2

>mess of proteins and molecules

Because proteins famously aren't molecules.