With the 12-person cell dismantled, police were hunting a 22-year-old Moroccan man, Younes Abouyaaqoub, suspected of driving the van used in Barcelona. They warn he could be at large outside Spain.
Investigators believe the terror cell comprised at least 12 men, some of them teenagers. An imam, Abdelbaki Es Satty, 40, is among the suspects, believed to have radicalised youths in Ripoll, a small town at the foot of the Pyrenees, where several suspects - including Abouyaaqoub - grew up or lived.
The imam has been missing since Tuesday.
On Saturday, police raided his apartment. They have raised the possibility that he died in an explosion Wednesday evening at a house believed to be the suspects' bomb-making factory, where police uncovered a cache of 120 gas canisters.
The suspected jihadists had been preparing bombs for "one or more attacks in Barcelona", regional police chief Josep Lluis Trapero told reporters, revealing that traces of triacetone triperoxide (TATP) - a homemade explosive that is an IS hallmark - had also been found.
Instead, they used a vehicle to smash into crowds on Barcelona's Las Ramblas boulevard as it was thronged with tourists, killing 13 people and injuring about 100.
Several hours later, a similar attack in the seaside town of Cambrils left one woman dead. Police shot and killed the five attackers in Cambrils, some of whom were wearing fake explosive belts and carrying knives.
The Islamic State (IS) group claimed responsibility for the attacks, believed to be its first in Spain.
A neighbour, 61-year-old French retiree Martine Groby, told AFP that four men "who all speak French" had been in the house next door since April.
"They were very discreet, too discreet. The shutters were closed, there was no music, no children, no women," she recalled.
Most of the suspects are children of Moroccan immigrants, including Ripoll-born Moussa Oukabir, 17, one of five suspects shot dead in Cambrils. His older brother Driss is among the four arrested.
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