66 Mhz and 33 Mhz are the default speeds of the AGP and PCI, respectively. You want to keep them as close as possible to 66/33 when overclocking (especially the PCI...the AGP can handle a good bit of OC'ing).
"An extremely useful feature with the fickleness of the AGP bus is the Async AGP/PCI CLK setting. This allows users to lock in a bus speed and will help maintain system stability during overclocks."
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