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Timothy Ray Jones Jr, 32, will be charged with five counts of murder, and officials believe he acted alone, Acting Sheriff Lewis McCarty of Lexington County said.
Authorities think all five children were killed at the same time, but they said they don't yet know how or why.
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Jones was charged with murder on Wednesday along with child neglect in connection with the children's deaths
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Jones was already in custody in Raleigh, Mississippi, after being detained on Saturday on suspicion of driving under the influence.
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Jones had joint custody of the children with his ex-wife following their divorce. He was their primary legal custodian, the Lexington County Sheriff's Office said.
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The murder suspect's father, Timothy Jones Senior, told
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today: I know my grandchildren are in heaven. I don't want no one to think that my son is the animal that they're going to put him to be.'
'This is a very tragic situation,'
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'These kids' lives were snuffed out before they had a chance to enjoy life. Justice will be served.'
He admitted to the killings in Smith County, Mississippi, after he was pulled over on Saturday at a driver's license checkpoint and arrested on charges of DUI and possession of a controlled substance.
Police have not released details on how the children died. The children's bodies were taken back to South Carolina for autopsies and identification on Tuesday night, sheriff's officials said.
Marlene Hyder and her husband, Johnny Hyder, said Jones and his wife moved into a house next to them about seven years ago in Batesburg-Leesville, South Carolina, 25 miles west of Columbia.
They said Jones told them he worked in computers. Two years ago, the wife moved in with a male neighbor and Tim Jones moved away with the children,
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Johnny Hyder said the children were often dressed in dirty clothes and were seen home at all hours of the day because Tim Jones had said he didn't believe in the public schools. Hyder said Jones was constantly looking for a reason to argue and often threatened to call the police.
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He said Jones approached him with a gun on his hip one day and was angry about something, but Hyder couldn't remember what it was. When Hyder said he was going to call police, he said Jones told him it was only a BB gun.
Marlene Hyder said Jones threatened to kill one of their dogs when it briefly went onto his property.
'He was a nut'.
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Mrs Hyder said she also remembered a day when one of the Jones' younger children came over to the Hyders' house and tried to drink out of one of their outdoor spigots.
He was dirty and disheveled and ran back to his house when she tried to speak to him, she said.
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Several people were seen walking around the yard, but refused to comment on the charge
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He said Jones led investigators to the children's bodies on a dirt road near the Oak Hill area.
The children's decomposed remains were found packaged in individual plastic garbage bags east of Camden, Alabama, said Smith County, Mississippi, Sheriff Charlie Crumpton.
Jones was detained Saturday at a checkpoint East of Raleigh, Mississippi, where police were looking for impaired drivers,
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The deputy found what were believed to be chemicals used to manufacture methamphetamine and a substance believed to be the street drug Spice, a form of synthetic marijuana
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