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I believe you are not activating the chip properly on startup.
For PSX disks, you dont need to use the GS - you already know that. However keep your finger depressed on the power button until the blue eject light flashes blue.
When booting up the GS, double tap the power button to turn the PS2 on. Try it a few times if it doesn't work.
If it doesn't work, try the same as booting PSX disks - leave the power button depressed till the blue light flashes on.
It is all a timing thing. As it stands at the moment, your modchip probably isn't being activated.
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