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One of the big cats fled when officers made loud noises, but the other animal appeared unafraid and continued to wander the area.
"The police chief made the decision that the cat had to be put down as it presented an ongoing danger to the community, especially in such close proximity to the Hannon Library, which was open at the time," the police department said in a statement provided to KDRV-TV.
A shot was fired, but it missed the cougar, which fled the scene, police said.
State wildlife officials said they are working with police to monitor the situation.