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.