Hi Daniel, welcome to the Forum.
I believe that it's very difficult to find the best h/r for a top just with calculations, because there are many interconnected variables which make the matter very complex, we don't even have all the needed data about air drag and tip friction..
The simplest way seems to make some different tops and directly test them.
Certainly there isn't just one optimal h/r ratio, because this ratio itself is variable, depending on other data, like for example the starting speed, the density of the material, the size of the top...
The optimal ratios you found empirically, between 1/2 and 2/3, seem high to me, probably the tops you used were littler and/or lighter than the mine.
Once I made three cylindrical brass tops, with three different h/r ratios, and external tip. The ratio of the best one turned out to be about 1/3,(weight 107 grams, diameter 59.9 mm, longest spin 26 m 20 s, by one twirl of the fingers). The tallest top was more efficient at high speed, but the flatter one had a lowest toppling down speed, and this made it spin longer.
You can see the test with the three cylindrical tops in this video: