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If you're aiming to improve memory speed, as well as size, I believe you'll need to remove the CL2.5 stick (or overclock it by manual timings if you can get away with it) in order to make use of CL2 speed.
So if you're adding a 512, and you have 256, you either go with 768 Mb at CL2.5, or 512Mb at CL2.
I presume we're talking DDR? as I've never heard of CL2.5 SDRAM
Also, the speed - if I've got it right....
PC1600 (obsolete!) = 200 FSB
PC2100 = 266 FSB
PC2700 = 333 FSB
PC3200 = 400 FSB
If you're motherboard supports it, and you might upgrade to a 333FSB processor, then investing in Pc2700 ram may be worthwhile, otherwise PC2100 may be cheaper
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