Yes, you can unassign a document that has been already assigned to a program until the closing of the application period (File Review). Simply go back to when you assign them and look for the checkboxes on the left. However, once file review has opened, you can no longer unassign documents.
Please note this is not the case for any Post-Match Process (PMP), as there is no file review period. Once an application is submitted during the PMP, it becomes available to the program. It then follows the same rules as though a file review period has begun.
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