Just started working on a cartridge emulator for 2600 using the Pico, code here:
https://github.com/sigmafx/atari_pico
Uses PIO to sample the address lines, interrupt to get the ROM data and PIO again to set the data bus.
For a 2K rom Pico was happy to run at stock 125MHz, but for a 4K rom I needed to overclock to 250MHz, not sure why, maybe memory access is too slow across the larger rom size??
I'm not going to finish this to a complete cart emulator, I just want to be able to quickly transfer roms to see the results of development work, so send rom over serial link and start execution. I'll put together a cart pcb with address line buffering for 5v to 3.3v - data lines work fine at 3.3v.