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On Monday, Belgian officials released a video clip from the museum's security cameras. It shows a man entering the building, taking a Kalashnikov rifle out of a bag and firing two rounds into a room before walking out.
The attacker left the crime scene on foot. "The priority of priorities is to find this man. He must be arrested and stopped," Home Affairs Minister Joelle Milquet said on Monday.
"We must reassure members of the Jewish community." She has ordered round-the-clock police protection at all of Belgium's synagogues, schools and cultural centres. Two of the four victims were Israeli tourists from Tel Aviv.
The other two were museum staff - a French woman and a Belgian man. All four died from gunshot wounds to the face and neck, the AFP news agency reported.
Deputy prosecutor Ine Van Wymersch said on Sunday he could not confirm whether the shooting was a "terrorist or anti-Semitic act". Israel's foreign minister and prime minister condemned the shooting, saying it was the result of "anti-Israeli and anti-Semitic incitement".