I for one, am planning to 86 one of my players characters in the months to come, using the opera aria "Vesti la giubba" from Leoncavallo's opera "Pagliacci", when the heroes are at the opera looking to save an important NPC from a ruthless assassin, only to find out too late, that one of them is in fact, the intended target...
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There are too many specific examples I can give, though I try not to use just one track for a scene - I usually make play-lists with music of the same style and mood for an entire scene or setting. I usually use OSTs and music without any lyrics.
One good example is the Silent Hill OSTs for scary/un-nerving/horror games. The 'calmer' tunes for the intro and the freaky bits for the haunted house/dungeon etc.
Another is to use a film score of a film that the players have seen recently and (most importantly) enjoyed. Eg. I used the Joker's weird theme tune 'Why So Serious' in a spy game when the PCs found out they were being manipulated.
Cheers! :D
My initial feel for that kind of set up would be the OST to Princess Mononoke, which has a meandering, adventuresome feel though not too frantic, with the demonic tracks saved for the NPC.
When the adventure comes to a head, drop in few of the tracks from the Spiderwyck Chronicles for the final crisis, when the trap is revealed (James Horner does good line of screaming crisis strings). For something more brooding, the OST for Alien3 is pretty good, and won't be as recognizable by your players.
My two cents, anyway.
It kinda depends on what we are gaming. I've never been a fan of pop music in the background, especially since my tastes don't equal most of my group's and the words are distracting.
I have pulled a few tracks from the opera soundtrack from Constantinople for Legacy of Fire. I also want to run a bunch of Lisa Gerrard's tunes from her albums, as they have a desert feel to them. She has several similar tracks on the Dead Can Dance albums. Loreena McKinnet has interesting eastern European tracks that sound like gypsy music that might work well also. Finally, Sarah Brightman's Harem has several Arabic-themed tracks to try.
Traditional soundracks for films have the unfortunate problem of volume-levelling, which is kind of unnerving if you aren't used to the particular album, so I shy away from them.
As for Xen'drik of Eberron, I've always wanted to run the Survivor theme. Corny, I know.
My co-DM is running us through RotRL. Given what we've encountered in the first part of "The Skinsaw Murders," I'm guessing I'll need to bring my soundtrack to Bram Stoker's Dracula with me next week...