So... why go through LLVM at all instead of having the MIR target PTX/HIP C directly then?

If they really wanted a vendor neutral solution for Rust GPU, that already exists: you write the CPU side code, including buffering, allocation, concurrency, etc through Vulkan binding and consume the compute kernel in SPIR-V from HLSL/GLSL/WGSL etc. As it stands, the way they use Rust here feels more like using it like TypeScript types/interfaces than anything else.

Again, the size of most operations that should be done on the GPU is known ahead of time before compilation, so it's very much possible to statically allocate memory at compile time instead of going through all this trouble to write what's essentially a Rust shaped DSL for GPU compute.