Windows Key makes sense, it's a command key that's not used by applications.
Ctrl + Alt are modifiers can be used on any key by an application most 105 keys. Shift is obviously more restricted as it shifts case, but it can still be used on function keys etc.
You can also combine those. Alt+Gr does have other uses too.
Probably what would be more useful, is a better custom binding tool for keyboards in Windows.


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