Have you tried to set the Key attribute to "LeftAlt" or "RightAlt" ? The Key attribute is of type System.Windows.Input.Key enumeration, which does not have an "Alt" value.
Alt used as a modifier in KeyGesture , so you see it separately in other places. However, in the key enumeration, it has instances for the left and right Alt keys.
You most likely should have two bindings, one for each alt key.
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