My thanks jiripolivka.
I have so far done what most of us do. We choose the lowest loss substrate we can, trading off the loss factor against cost, ease of use, etc. For example, I choose some that have some ceramic loaded in with PTFE because vias can be made without a difficult sodium etch needed to adhere the metal. The dependence of frequency is a refinement we usually do not go to because Er and tan(delta) are normally fairly constant over a usual band of interest.
This time however, I was trying to model radome-type surfaces, not used in a circuit-building context.
I (think) I found the way. A description of how to use a couple of known values to establish at least the simplest order Debye rule for the material. I will hold off posting anything about it yet until I am reasonably sure I have got it figured out.
Meantime, I had hoped someone had gone further than entering only one Er, and tan(delta) when supplying material properties. Mostly, one is able to avoid even that, by just choosing a nice substrate from the default list.