I mixed a medium gray, some plain yellow, and some burnt umber from those small plastic vials of acrylic crafts paints you get in the craft section at Wally's. The ratios would be four, 1/2, and one, mixed, and then diluted with about four times as much water. You are making a very heavy wash because you don't really want to 'paint' as much as you want to 'stain' the plaster or hydrocal casting.
I found that one application was lots. Adding another would merely darken the 'stone'.
Next step is to blacken the grooves between the stones. You need a wash for this. You take plain black in acrylic paint, dilute it in a ratio of at least 8/1 with water being the greater component. Dip your brush and wash this solution liberally down the stones starting from the top. Move it down ward and let it settle in all the nooks and crannies. Then leave it, set on its flat back! You want it to settle and dry in the grooves. Not dark enough? Repeat.
Lastly, you must create the soot over the arch and on the side frame. Tale some of that black wash and add a bit more black paint to it. Now you want a heavier wash. Dip a clean brush into this heavier mix, and squeeze most of it out, and then swipe a clean paper towel three or four times to get most of the wash out of the brush. Then you start to blacken up the apex of the arch and the side-walls. Let it dry, and add more to the central dark part, right over the keystone or whatever, to concentrate the soot effect. Keep doing this until you get a look like what appears below.
Important. To get that gee-whiz look to what lies behind the portal, take some time and create a block from view to any wood or white plaster, pink or blue foam may be visible to visitors and yourself. Create a tube of sorts that runs at least five or six incheas back and blacken it thoroughly. Then glue your portal in place.
I painted my portal first and then placed it. At one point I added a bit more wash to darken the soot, but by then the item was hard in place and could be reached and modified with a paint brush easily.