难忘那迷人的普陀山 is translated as "THAT hard to forget bewitching/enchanting/fascinating Mt. Po Luo". Same usage as in the English "that" to emphasize that particular mountain. You cannot substitute with 和 which means "and" and if you want 和 to mean harmony, then you must add another character to distinguish from the conjunction meaning. However, it becomes too wordy and did not suit the intent of the original thought.