I think you will find that a new video card will help you more than what ram would as far as FPS goes. Sure the ram will help with the speed of your PC but it doesn't make a great deal of difference when it comes to FPS.
Good choice for sticking with ATi as they are a better card and have better driver support. As for which card to choose. That depends on how much you want to spend.
Also don't be put off buy purchasing a card that requires power from a power supply. As power supplies have come down quite a bit over the years and good quality power supplies are not that expensive. Plus the performance you will gain from a higher end card that requires the power will be exceptional.
I have a GeCube 4870 with 1GB ram in my gaming PC and it really moves. I play lots of Call Of Duty when I can and there is never an issue with FPS or performance from this card.
Even with SH3 and all my mods enabled I still manage to get between 300 - 440 FPS depending on how much action there is. But my FPS never drops below 300 even in the heaviest combat situations.
Anyway that is something to consider and if you let me know what your budget is I would only be to happy to help you further in deciding on what card would be best.
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