Since it is ultracal, you’d want to use a soft material like silicone, backed with a support shell.
There is a vast number of silicone rubbers and support shell materials you could use, but if you wanted to do it super easily and quickly, you could buy the Body Double silicone trial kit from smooth on, and some fast set gypsum bandages. Build the silicone up in 4-5 layers or however much you can get away with using the kit, and then use the bandages to make a two piece support shell. Depending on how far back the mold goes, you may be able to get away with a one piece shell, but for safeties sake, I would recommend splitting it into two. I would split it down the middle of the face, lay one half up right on the center line and then release the edge well. Apply the other half slightly overlapping that first edge. Let it set, remove the shell and silicone, and you should have a good mold. Alternatively you could use something like rebound 25/40. It would give the mold a longer library life, but it also extends your molding time by a few hours.
I like to use dish soap as a release when I cast silicone into silicone. Ivory soap in particular. Adding a little 99% isopropyl alcohol will stop it foaming.