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After completing the Waters of Life quest, you will be able to pick up a broadcast when you are close to Vault 101 (Megaton seems to be on the very edge of the radius). Tuning into the broadcast will start the "Trouble on the Homefront" quest. Be aware that once you complete this quest, your access to Vault 101 will be permanently revoked, so make sure you've gotten anything that you can't otherwise get elsewhere (the Medicine Bobblehead, Rock-it-Launcher schematics).