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Belgium launched a nationwide manhunt Sunday for a lone suspect in a shooting attack at the Brussels Jewish Museum as the toll in the attack rose to four dead.

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The attack, which came on the eve of national and European Parliament elections, led officials to immediately raise anti-terror measures and increase the protection for Jewish sites.

Video of the attack showed an athletic man with cap calmly walking into the Jewish Museum, getting out a Kalashnikov shoulder rifle and starting to shoot before briskly walking away.

No one has claimed responsibility for the killings.

“We call on the whole population to help identify this person,” deputy prosecutor Ine Van Wymersch said Sunday.

She said the gunman who killed an Israeli tourist couple, a French woman and a Belgian man with shots to the face and throat “probably acted alone, was armed and well prepared.”

The fourth victim died Sunday afternoon, said a government official who asked not to be identified because the news had not yet been officially announced.