It's so hard to choose, but I would have to say the North Karana bridge music. I'm not sure that that was the original intention for the music - it might have been for Dagnor's Cauldron or some such.
In any case, I was on my first character, a barbarian who spent most of his time in Blackburrow and never ventured much past Qeynos. My friend had just gotten the game and rolled a wood elf. I stocked up and planned to make the trip from Halas all the way to the other side of the world. I was going through the karanas and had gotten lost - all I had to go on was maps printed out from eqatlas. Having already had the horror of falling down the trap door in Blackburrow, I couldn't imagine dying way out in the Karanas. It was raining so I couldn't see much at all due to the fog so I was just trying to follow the road. After a while, the rain clears up, that ominous music starts playing and I see this giant epic wooden bridge leading me on to where I was headed, both the sight and the music seemingly warning me of the dangerous journey that I had barely even started as I approached what I only knew from a map as Highpass. Easily one of the top moments in my gaming history.
Also, that cottage music in North Ro is definitely an awesome and memorable song. My friend and I were doing a trip from Kelethin to Oasis as we had gotten too high for Crushbone (this is on P99, like, 2 days ago lol). He's got me on follow as we're going thru North Ro and I just stop and I'm like... man, I have to just listen to this music for a minute, wow. So good.
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