This song was in Breaking Bad's season premiere on Sunday (you know, when Hank was hard at work in the garage), and I tried to Sound Hound it with no result. Then I came across this Vulture interview with show creator Vince Gilligan where he talks about the song by his former schoolmate, Jim White.
Bonus: Here's another one that struck me during the show. This was during the second to last episode of season 4 when "Walt sits at home, alone, with his 38 snub at his side. He mulls over his options, spinning the gun three times on its side as he does so. The first two times the barrel of the gun stops pointing straight at Walt, while the third points at his nearby flowerpot." (thanks internet nerds.)
And one more...Madrigal. Walt and Jessie search for the ricin cigarette.