I'm pretty sure they tried this at MIT a few years ago... overclock an ancient processor by overriding the BIOS and going straight for the cold via super-cooling. I remember reading an article about that back in 2002 or so. I think a few of their teams were able to get them up to 1 GHz or so... but there's a few issues you'll need to recognize immediately before attempting this:
1. Cooling. Shy of building a space ship and flying to Pluto's surface and trying this outdoors at night in Pluto's winter, the cooling is going to be extremely hard to do. The faster the processor computes data, the hotter it gets... most modern processors are built for overclocking and won't let themselves speed up beyond a PNR. Older processors however aren't like that, and that's why the 386/ 486 era of intels were the golden redneck age because people back then were trying all sorts of wacky stuff to overclock processors. If you have access to something like liquid nitrogen, give it a try... why not
2. Bussing. The old processors couldn't bus information like modern ones, and unlike overclocking the processor speed, there's nothing you can really do about that. So even if you do manage to get the processor up to 1 GHz or beyond, the true effective speed will be hindered by it's relative slow bus speed.
3. Old processors aren't designed for modern multitasking. Back in the day, you ran one program off of the big black 5.25" floppy drives at a time... you couldn't play a game and have calculator and notepad underneath them running at the same time (especially considering that those things didn't exist. I don't know if an old processor, even if overclocked, can multitask like that... can it?
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