New Alexandria. Although personally, I'd go with Lone Wolf. Both were concepts not done in a Halo game before, and Halo 4's attempt at the first one was...
I'd say the stretch of Long Night of Solace, Exodus, and New Alexandria felt pretty good.
New Alexandria was a good mission, but I wouldn't quantify it as hallmark Halo. It's certainly unique and I love the free-roaming gimmick, but it needed more on-foot stuff to do. It was like a sampler platter of three small missions and a proof-of-concept for a bigger hub area all polished up and given sub-objectives. They should have at least given us more Banshees to face, or made them more aggressive. Even on Legendary they're pretty casual about the whole "kill all humans" thing.
Lone Wolf is kind of in the same boat. Thematically it was a great way to convey the end of the game and put a resounding period to the game. Playing it, however, has no real impact. You just hold out till the end.
The reason The Ark and The Covenant are so great is because their design meshes very well with the sandbox. Reach is a bit too limited to really drive home something like NA with the Falcon being the primary signature of the mission. Some adjustments to Banshee AI would have really helped it, I think. That and more on-foot stuff to do. It's also a pretty quiet mission, which I like. But the best missions in Halo have typically been louder, more convinced of their epicness.
Like Tip of the Spear. That one screamed "greatness" at the top of its lungs...and instead, we got middling. I'll still look at their massive battle prototypes built in the Halo 3 engine with nothing but bitter tears.
Are you forgetting the mission where you fought Covenant patrols as buildings crumbled around you and cruisers began to glass the outer reaches of the city just in time to fight four Hunters in a nightclub?
Was it cool to fight the Hunters? Yes. But it did a poor job making that a centerpoint moment. It just sort of happens, just like everything else in that mission. A little bit more Marty magic would have made it a lot more memorable. That and the fact that most of the time the Hunters only fight you two at time really nix that part of the mission as "holy shit" and make it more like "oh, that's cool, I guess."
And that's the problem with Reach. "That's cool, I guess" is what propels most of the game, despite it having some really solid level design and some great ideas.