Maybe not what you are looking for, but Quinton Tarantino's soundtracks-especially for "Pulp Fiction" and "Jackie Brown"-certainly set a certain type of vibe.
Once we get rid of Gladiator, PeterGabriel and Vangelis, top spot for "moody" musik goes to David Lynch CDs (yes, of Moolholland Drive fame). Sublime and deeply disturbing... Nils Petter Molvaer soundtrack is almost as good as his "Khmer" masterpiece.
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