My three picks, although all of mine are laced with more of an element of ‘hopelessness’:
Hero Core - Tetron
Demon’s Souls - Flamelurker
Lagoon - Walking in the Shadows
A little context on that last one: you start out in the first town which has just the happiest lil theme ever, and when you’re done with whatever stuff you’re supposed to be doing in the town, the game suddenly kicks in this urgent sting and you discover a dude damn near disemboweled at the town outskirts. Then you wander into the nearby cave and the music above, the soundtrack to your first combat experience in the game.
Love this song from the Mother 1 town where all the adults have vanished, leaving the children alone. Sad, mysterious, and anxious vibes. Sounds like the soundtrack to an Unsolved Mysteries episode or something.
Xanadu Next main town music. I’d describe this as cautiously hopeful amidst danger:
Darkstone main town music. The sound fx do a lot of work here but the melody is wistful to me:
Eternal Eyes music that i think plays during cutscenes. I would again describe this as wistful. It sounds straight out of chrono trigger as well to me:
I’ll have to think some more and see if i can come up with some older examples that other folks haven’t posted.