Peter Manfredonia, 23, had been the subject of a six-day search involving several police agencies and the FBI.
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He was found in Hagerstown, Maryland. He was not injured and no officers were either during the arrest, police said.
Manfredonia was wanted in the machete killing of 62-year-old Ted DeMers and the wounding of another man in Willington, Connecticut, on Friday.
The University of Connecticut senior also went to another man's home, held him hostage, stole his guns and truck and drove about 70 miles (110 kilometers) southwest to Derby, Connecticut, state police said.
In Derby, police found Manfredonia's high school friend, Nicholas Eisele, 23, shot to death in his home on Sunday. Authorities believe Manfredonia then forced Eisele's girlfriend into her car and fled the state. The girlfriend was found unharmed with her car at a rest stop near near Columbia, New Jersey.
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Pennsylvania police said Manfredonia took an Uber to a Walmart in East Stroudsburg, not far from the New Jersey border.
Police discovered through interviews with the driver and from security camera footage that Manfredonia walked behind the store and onto railroad tracks, authorities said.
A man fitting his description was spotted Tuesday night near Scranton, Pennsylvania, prompting another search there. And police later suspected Manfredonia to be in the Hagerstown, Maryland, area, where a ride-hailing service dropped off someone matching his description Wednesday.
A lawyer for Manfredonia's family said he had struggled with mental health problems, but did not show signs of violence.
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