Ultima Underworld 1 & 2 without question, from the available options to pick. Excellent quality duo of games, had lots of fun with, and time spent on these. However if there was possibility to pick more than one I'd choose Lands of Lore also, because of it's great mood. Of course, it's all just my personal opinion.
I also agree Betrayal at Krondor would be an excellent choice to pick here, played it quite a few times and it's story, and music (if CD music on CD version) are great and really well done.
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