The best time (that did NOT involve sending somebody flying off a tower ledge/mountain peak) was at the Hag's Cure in Markarth.
Bothela caught me stealing something off the shelves, and wouldn't relent on slicing me with a dagger. I was just backing away trying to figure out what to do - when I backed up into that adjacent bedroom with the 2 beds and table up upon the raised area.
I just said to her "Are you SERIOUSLY going to do this?" and then switched to my Unrelenting Force and gave her a full-force blast.
The results of which I will never forget.

My Fus Do Rah sends her flying straight-backwards, right over her shop counter and directly into the shelves behind the counter. She literally slams her full-body back-first into the potion/ingredient shelving. As soon as she hit the shelves - EVERYTHING on the shelves blew off and scattered everywhere! It was LITERALLY like a scene out of some action movie like Terminator - where you see some guy get thrown across the room and through a huge display case by a Terminator.
And the icing on the cake? After she gets up and all the bottles/ingredients settle and stop spinning - instead of continuing the attack, she screams and runs out the door.
I couldn't stop laughing for a half-hour... and I could NOT have scripted that sequence any better.
