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Since the song you heard is on "Hypermagic Mountain," I recommend that as a starting point.
If you absolutely love it, then your next LB purchase oughta be either the "Power of Salad & Milkshakes" DVD or the "Wonderful Rainbow" LP/CD, then go back and get "Ride the Skies" and (if you must have everything ever) finally the first CD, which I'll warn you is really roughly recorded and only valuable as a document of the band's earliest activities.
The DVD is actually better than any album, as it captures the band doing what they do best...playing live to small intimate audiences. Now that the band's popularity has built considerable critical mass, it's not gonna be the same for new fans of the band as it was for us older fans who saw them play in small basements, living rooms, sketchy warehouses, barns, and places like that.
I was lucky enough to have Lightning Bolt play my living room here in Davis back in 2001. They were so tremendously loud that people's ears were in pain, yet the whole vibe was so blissful, no one ran out...the music just sucks you in. That was perhaps the sweatiest my house ever got. The eerie red-lit footage in LB in the DVD is from my house. Pink & Brown and Total Shutdown also played that, and it was also the first ever public performance of the band Hella.
As a tour documentary, this DVD works extremely well. Even my mom was not able to look away from it despite the music being beyond her realm of what is actually music.
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