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I vote for Little Green Bag. Sure Misirlou is a great song and really evocative of the movie - but once they pull that gun in the diner, it cuts to straight opening credits. You don't get something happening during the song itself like with the side on/straight ahead filmed slow mo walking, cigarettes, suits, lethal raw machismo in the Reservoir Dogs opening. Watch it again, a truly awsome sequence. There's a reason it's the logo for A Band Apart productions.
Have to say, while it didn't strike me during the movie, I love listening to Goodnight Moon on CD. It's such a damn sexy, slinky song.
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