3 600 MCM copper in 1 conduit is kind of an odd set up... 420 amps ampacity is well over what a 400 amp breaker can carry continuously, it is 80% of a 500 amp breaker, (though I do not know if they make such an animal), the run is not so long that voltage drop should be that much a concern... again, what ampacity do you need, and what size breaker are these coming from?
675 ft of copper versus aluminum.... may wind up close to a wash by the time a second 3.5" ENT conduit is run and extra-time terminating is taken into consideration.
Eta: looks like you can pull up to 8 400 MCM wires in one three and a half inch conduit, so if another Raceway isn't needed, aluminum will definitely be the way to go here