For this shot, I think you could have gone a little more oblique with the key and had it further behind him and the at would give more edge to the cheeks and let the shadow of the eye socket wrap around the brow a little more. That in turn would darken the inner portion of the eye socket then you can bring you fill down some and catch the eyes a bit without losing the moodiness. Ratios look good though. With the key further back behind you might be able to eliminate the fill light and replace with a reflector and you wont have to worry about getting low enough power. Shooting at f22 that probably isn't an issue though.