When does the union break up?

What if the constitution had a provision for a state to wihdraw from the union?
It could be by 2/3 vote of the state's legislature.
When would the union break up?
Would it be replace by an alliance of states?
 
Could this have happened? The Articles of Confederation were replaced by the Constitution to create a stronger government. But how strong could the Federal be if states could walk whenever they wanted? Maybe the method of leaving would need to be more complicated, and delayed?
 
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