There are some who will swear by s06e10 and s06e11 "Chain of Command" as among the best. I haven't included these because the scenes of Picard's torture were too disturbing for me. And the villain didn't even die, which is the least I would expect at the end of such stories. But yes, the double episode had its moments, and one of the best was the change in Deanna Troi's wardrobe. She's smartly dressed from this episode on.
See also my posts on Captain Picard's Finest Moments and The Most Attractive Women of Star Trek TNG.