Hey, I see nobody else stepped up to answer, so I'll take a stab.
As far as I know, PICO-8 itself doesn't give you that option. But there two ways to tack it on afterwards.
The other solution would be hacking the exported JS file that represents the cart - the core logic of binding keyboard to PICO-8 buttons lives in there, but it'd probably be very annoying to try and do it this way (and any hacks you do would be lost on re-export).
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