What do you mean by something that didn't yet appear in games, btw? I'm a bit confused by this line...
You have pretty much answered yourself saying "Its psychological dimension was very realistic as well as charming! And some scenes in the series were almost done in an experimental fashion".
Oops, seems I have xD Actually, I think The Path managed to do that in a way. And Team ICO. Definitely what I'd call unique, fresh and personal.
And since this topic is about a Hideaki Anno's movie, maybe you'd be interested in watching Shiki-Jutsu? http://www.youtube.com/watch?v=32WdNraeZwE Haven't done it yet myself, but darn, it does look interesting.