I had mine running my 24/7 overclock, then used AI suite to raise it. That's just how I did it. I'm sure there are a lot of different ways, but it's just what works for you and your board. AI suite in turbo Evo, won't tell you your offset, for example, it will just tell you what the current voltage is in BIOS. For example. I run 4.6 every day with an offset of -.020. When I open Turbo Evo it will tell me my Vcore is 1.030. Then I take it from there. Increase your Vcore to what you want then apply it. Then change the multiplier, making sure the group cores box is checked, and apply. If you try it the other way around, you will BSOD right there. Just a suggestion. Keep a log of the frequencies you run and what vcore they were. It will make a good reference for later when you want to play some more.
EDIT: Tommy another suggestion. When you start the overclocking, go to Device manager and select properties on your Windows 7 drive, go to properties > policies and uncheck both boxes. Then,I've been told if you BSOD it won't corrupt your system files. When you finish, change it back. Also, whatever you set in AI Tuner will stay that way until you reboot. When you reboot it will revert back to what you have set in BIOS. If you are in AI Tuner and find a good overclock you like, save the profile. Name it whatever you want. Then you can open the AI Tuner and select the profile and load it, without making a bunch of changes.