Definitely up the CPU Voltage. How you do it depends on your style. I like to start out at 1.4v. If I'm stable, I work my way down. Other people like to slowly work their way up until their stable. Either way works. When I find my lowest stable CPU voltage, I increase it by a hair to give it some headroom.
I checked out your RAM. Its default voltage is 1.8v. So for now, I would leave DDR2 Voltage on Auto.
Actually, what you should do is drop your multiplier down to 6 and explore how far you can push your RAM by increasing the FSB. The DS3 overclocking guide on [H] suggests that you do this first. The advantage of doing this is you find out at about what point your RAM becomes the bottle neck. During this process, you may want to up the DDR2 voltage.
Another thing to keep in mind is that you can always drop your multiplier. You may discover your RAM can handle a FSB of 400. So, 9 x 400 is 3.6GHz. If you CPU or cooling can't handle that, then dropping your multiplier to 8 still gives you 3.2GHz.
I upped the pci e frequency to 102, set pci e overvoltage control to +.01, fsb overvoltage to +0.1, mch overvoltage to +0.01 and move the cpu voltage up to 1.4v.
So after a few days of different tests I find myself stable sitting at 2.925 Ghz with only upping the cpu voltage by .05. After running orthos for 6 and 1/2 hours I reached temps of 62, is that still considered stable? I was mainly sitting between 57 and 62 for most of the test.
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