See my recently initiated thread on the 4 sticks of Crucial Ballistix DDR2-1000 modules.
I'm still trying to sort this out.
Experience has told me that you need to re-certify over-clock settings if you add additional parts to a system build. Ideally, you'd have all the parts put together before tweaking the system, but -- even for someone like me who has learned already to suspect such to be true -- it just doesn't work out that way.
On the matter of filling two slots versus four, you're better with two. There is a bigger chance, given the quality of the memory you're using, that you can run the memory at a 1T command rate with a single two-module kit, grabbing some extra bandwidth in the process. And conversely, filling all four slots will nearly assure a need to loosen the command-rate to 2T.
My intuition tells me also that you may have to loosen the timings on a four-slot configuration. I was hoping that it wasn't so, but I'll certainly comment in my own thread if it turns out that the ORTHOS errors disappear with slightly loosened timings.
The errors that I chronicled in that thread occur with these high-performance modules running at 667 Mhz (DDR) and 3,3,3,6,2T. I'm loosening them to 3,4,4,8,2T to see if that resolves the difficulty -- before I pull out the last-added 2x512 kit and send them to Crucial under warranty.
This also means -- if the timings DID need to be loosened -- that my timings at a higher over-clock will need to to be reset to something like 4,4,3,8.
We'll see in about three hours, and I'm interested in comments from knowledgeable luminaries who want to post on either thread.
For the moment, I think others will confirm that you either get higher performance in memory operations at the expense of less memory (and lower performance from what it implies in the system storage hierarchy), or lower performance in memory operations with a gain in memory size.