Select esim_led from eSim_devices.
The components from eSim libraries are compatible with Ngspice.
If you add any diode, transistor or component present under eSim_Devices, then those libraries will be present at eSim-1.1.2/src/DeviceModelLibrary.
Now, since you have used LED (present in Diode folder in the above path) then when you click on "KiCadtoNgspice", under Device Modeling tab, select and choose where you have saved LED/Diode. That is eSim-1.1.2/src/DeviceModelLibrary/Diode/(select D.lib or LED.lib)