Size doesn't matter, demeanor and technique does.the older rooster is an ISA Brown, and he is quite big is that still okay?
A good cock/erel, no matter his size or age, will not try to mate a female that is not in, or close, to lay.
There's no telling, form what little info we have, how the 2 males will act around the hens and new pullets. Multiple males can often create chaos due to competition.
Were these two males living with the 3 hens before the pullets came along?
How do the males get along, do they fight or over-mate then hens?
Your 150sqft run is just big enough for 15 birds.
Wonders how big your coop is.