2. I'm not aware of good learning resources. Explore existing such code, e.g. opencl miners tend to use asm. Read in amdgpu/ in LLVM. Disassemble code from OpenCL and read the ISA. Explore and experiment, but it's tedious. I would not recommend to jump into ISA initially. BTW AMD does have good GCN ISA docs available online, that is useful!
3. Yes I often read the compiled ISA, and over time I discover bugs and also better understand the ISA.
4. OpenCL is SIMD, and yes it matches the GPU HW.
5. most important is to reduce the number of registers used (#VGPRs), as that influences heavilly the occupancy of the kernel. Use fewer costly instructions such as FP64 mul/FMA. Sequential memory access, and in general reduce global memory access as it's very slow. Merge small kernels into one (keep the data in the kernel). Never spill VGPRs.