Here's a thought. In an alternate world where gameplay didn't matter and the main storyline was just a footnote, which games would you consider the best in terms purely of the atmosphere and feel they manage to convey?

Some examples for me would be Breath of the Wild, Tales of Symphonia (obviously), Persona 3 & 5, A Short Hike and arguably some horror games like Silent Hill 1-3.

Persona 3 is a great pick.

But I think that would be Diablo.

Literally descending a church undergrounds to get closer to hell and eventually fight the lord of the demons. Not to mention Tristam and its ridiculously atmospheric OST as well.

For various reason come to mind: Mafia 1, Nocturne, Beyond Good & Evil, Privateer 2, Okami, S.T.A.L.K.E.R. and of course Max Payne 1&2
(Obviously most of those are great also in story/gameplay, but still, best atmosphere.)

Metal Gear Solid, Shadow of the Colossus, Silent Hill 1 and 2, Resident Evil Remake, Parasite Eve, Chrono Cross, and Devil May Cry.

Edit: and of course Bloodborne.

Super Mario Galaxy

Immediately what comes to mind is Warcraft 3 (and by extension, WoW) and Halo: Combat Evolved.

Shadow of the Colossus and Ico.

Wait, so is Diablo a game that Christians should be ok with then?  For any other Christians, would and do you enjoy slaying the devil?

I haven't played a VR game in several years, but there were quite a few just immersive cool atmosphere games on the first PSVR1. I liked Resident Evil 7 on the tv, but playing it in VR was just another level I didn't think possible at least not anytime soon. The shark demo that came with the system was really immersive. Not a good game and it made me dizzy playing it after a while, but Here They Lie had quite the atmosphere and felt like walking through a post apocalypse world. Thumper VR was another one, rather simple but in VR was just so much fun and so immersive.

Breath of the Wild. There is simply no competition.