Zinskaro; with clips of Nosferatu 1979 on Youtube
Lots of good thematic music in (wait for it) a number of the Castlevania games.
I'd particularly suggest the soundtracks for Curse of Darkness, and Lords of Shadow. Lament of Innocence, Order of Ecclesia, Portrait of Ruin and the rest all have good selections. It just depends on what the exact tone you want is.
Some of my favourite.
Sarabrande of Healing from Curse of Darkness makes a good, melancholy, "bitter sweet" moment.
Belmont's Theme from Lords of Shadow makes a good "prepping for the final confrontation" music. Perhaps after some terrible act spurs the players to action and enter "The Castle."
Love Lost from Lords of Shadow would work extremely well for one of the NPC's in the first dungeon, and Final Confrontation, also from Lords of Shadow works extremely well for... well, Final Confrontations.
I'd also suggest The Woods and The Goddessand York and Zach from the game Deadly Premonition, both of which make good background music from when things are a little more peaceful.
Finally, if you're looking for something a little more modern that gets the blood pumping and you don't mind vocals, I'd suggest War by Poets of the Fall, which is in their Twilight Theater album and the game Alan Wake.