There are reports of severe performance degradation in XP, due to misalignment, read/modify/write operations causing missed revolutions of the platter, etc.
I'm running Win7 on my hardware Windows boxes now, but if I were still running XP (other than VMs) I wouldn't use these >2GB drives for anything but archive storage.
yeah, I hate having 2GB drives, too :)
Specifications for the WD Caviar Green (Advanced Format) SATA internal hard drives
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