Around 200 police officers are involved in the operation amid growing fears the child may have come to harm.
Constance Marten, 35, and Mark Gordon were arrested on Monday night in Brighton but the two-month-old was not with them.
Detective Superintendent Lewis Basford, of the Metropolitan Police, said they still hoped to find the child safe and well, with a helicopter, tracker dogs, thermal imaging cameras and drones being used in the search. However, he said police had to consider the possibility the baby had "come to harm" as the couple refused to reveal where it is.
A member of the public phoned 999 after seeing them withdraw cash from a convenience store in Hollingbury Place shortly before 9.30pm.
Officers arrived six minutes later, with Marten and Gordon being detained on suspicion of child neglect and later gross negligence manslaughter.
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