I know you can make custom toolbar buttons that can be 'armed' by right clicking on them, and stay armed until you click again, and you can also assign this arming action to a keyboard shortcut, so that's very nearly what you're after. I assume you want it to only be active while you're holding down the modifier though, I'm not sure this is possible, but the solution I just mentioned is only one extra click - one to arm, and one to disarm, as opposed to just holding down the one key which is what you're after.
Kenny has a video on creating custom toolbar buttons if you're unclear on that. Once that's done I believe you make a cycle action for arming/unarming it, which I think Jon has a video on.
Bear in mind though that you can assign the mouse modifiers (ctrl/alt/shift) to any action in the preferences menu, so I have alt+click assigned to split, and alt+shift+click assigned to split ignoring snap, so that might be a faster way of achieving what you're after, without using toolbar buttons at all.
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