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The Enclave weren't just randomely killing off the Vault Dwellers, they had a reason.
The Enclave started scouting all over California with their vertibirds and establishing a base at Navarro after the Vault Dweller defeated The Master in 2162. Then when they saw all of the remnants of The Master's army and the ghouls, they decided the "mutants" would have to go, including all of the humans who had been exposed to background radiation after the war if they ever hoped to inhabit the mainland again. They found the Mariposa Military Base, and excavated it, and got samples of the FEV virus, which they could turn into a lethal toxing that could kill anybody who wasn't first inoculated against its effects.
The Enclave needed two test groups: one of clean, pure humans and another composed of the "mutants" that lived all over the mainland, suffering radiation and FEV exposure for decades that, to the Enclave, made them unclean. The unclean sample was easily obtained by kidnapping the entire population of Arroyo.
The clean group would be more difficult to obtain though. The Enclave wouldn't allow the Chemical Corps to use people living on the oil rig so they had to look elsewhere. Thus, they traveled in force to Vault 13 and sent a command to the Vault's computers to open the Vault door. After taking care of some mild resistance (after shooting three unarmed vault dwellers who came to greet them), the Enclave troops rounded up the residents of Vault 13 and shipped them off to the oil rig in Vertibirds to take part in the Chemical Corps' FEV experiments.
And that is why The Enclave went to Vault 13 in the first place, and killed whoever they felt were "resisting".
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