You can certainly do it with ePSXe. Use a graphics plugin like Pete's OpenGL2 and it has a raft of options that will display the graphics perfectly in full screen, it will also use your videocard to anti-alias it if you like, making the game look more like a PS2 title.
PSX uses far more faithful 1:1 emulation so doesn't employ any graphical trickery, meaning full screen (especially on a widescreen) and high res will tend to make the game look like a dogs dinner. PSX only really works well in a window or displayed on a proper CRT TV.


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