Hard to say what’s the absolute best one, but some highlights:
Finale of Ace Attorney Justice for All; when you finally have the change in circumstances needed to pin the real killer and send them into a genuine panic.
Pizza Tower, final boss third phase: When Peppino sees that Pizza Face is sending him a Boss Rush, and flips his shit, annihilating each boss at lightning speed.
Ghost Trick, Phantom Detective: The final “4 minutes before death”, and multiple last revelations
Most of these are memories of story-driven moments nailed in by very solid soundtracks, which has very much convinced me how important music is to these games.