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Aenima is their most popular.
Undertow is their first full length, but it has some "metal" types of moments atypical of most of their work (i.e. the thrashy burst in the middle of Crawl Away-but it's cool for that song).
Lateralus and 10,000 Days are awesome too, but they might be a bit difficult for a beginner.
So, I say Aenima.
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