As you are new to Young's music, After the Gold Rush is perfect for you. It's exactly that country, folk-rock style that Young is playing almost all the time, and it is very very good, the first 5 songs are just fantastic. Then, of course, the Harvest Moon precursor, Harvest - my absolute favorite Young album. It is a little bit stranger, because of songs such as "Words" which is very psychedelic-orientated, but it's soo damn good. If you find Harvest first, buy it, you won't be disappointed at all, it's just that there are 3-4 songs that aren't this folk-rock style, but every song on the album is just magnificent.
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