Hm. It's a tossup between the first and the second, I think.
Takamine's group adds an interesting layer to the first game - they're painfully aware of what's happening to them and desperately trying to solve it, just the way Miku is. It's also the only game where some of the ghosts seem to have some degree of self-awareness - Takamine showing Miku where an item is hidden, and Munakata trying to tell Miku not to be afraid during that boss fight.
The second game is the most emotionally involving, though, with the excellent flashbacks and the Spirit Stone Radio, and the way it demonstrates just how damaging the ritual was to the survivors.
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Takamine's group adds an interesting layer to the first game - they're painfully aware of what's happening to them and desperately trying to solve it, just the way Miku is. It's also the only game where some of the ghosts seem to have some degree of self-awareness - Takamine showing Miku where an item is hidden, and Munakata trying to tell Miku not to be afraid during that boss fight.
The second game is the most emotionally involving, though, with the excellent flashbacks and the Spirit Stone Radio, and the way it demonstrates just how damaging the ritual was to the survivors.