I've yet to form a definitive opinion on 4,5 and 6 because I've only played half an hour of Last Revelation and frankly, glad to be past the kiddie training level. I've played 5 hours of AOD and I've only just reached level 4 out of 29, which is roughly how long it's taken me to get used to the controls.
Chronicles, I haven't touched yet.
But I can say that 1, 2 and 3 were always my favourites and I finished them several times over down the years and am loving those remasters. The grid controls are now second nature to me in those games, so one could say that AOD is a bit of a hybrid.
As for LAU, I'm not sure if they need a remaster, especially Underworld, because it still looks great in my opinion.