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For ambience, post-rock works really well. This might be pushing it, but for unsettling dark sort of tones I'd go for some John Murphy. He does a lot of soundtracks, but my favourite is easily the soundtracks for the 28 Franchise. Check this. Olafur Arnalds does some great stuff, too, though that track in particular might not fit entirely. Aidan Baker does some cool alt/experimental/indie stuff that gets pretty dark. I'd recommend browsing through his stuff to find something suitable.