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Nick Cave - Tell Me What That Is from the Wind River soundtrack. It’s more sad and unsettling once you know the context and what happens in the film.
So many cool suggestions in the comments, I have to add a mention of Ennio Morrricone’s soundtrack to “The Thing”.
On a personal note, Shnitke’s Concerto Grosso #1 always sounded like a manic bad dream to me.
I had this discussion with a class the other day. It doesn’t answer your question really, but the Requiem for a Dream soundtrack is rather unsettling if you’ve seen the film.
Can confirm, it’s very emotional.