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The minute U.S. troops reached Osama bin Laden's compound in Pakistan, they set in motion not just the takedown of the world's most-wanted terrorist, but also the largest potential intelligence coup of the post-9/11 era.  

Putting into action a specially designed Sensitive-Site Exploitation plan, the Navy Seals who conducted the raid carried off five computers, 10 hard drives and more than 100 storage devices, such as DVDs and removable flash drives, U.S. officials said.  

The intelligence find is a jolt to bin Laden's network that could force its terror operatives to move into areas or initiate communications that make them more easily detectable.  

A Central Intelligence Agency task force, which has already conducted a preliminary analysis of the material, is hunting for leads on the location of bin Laden's second-in-command, Ayman al-Zawahiri, who is widely expected to ascend to the top of al Qaeda, as well as information about new plots, names of other terrorists and any information about whether members of the Pakistani government helped conceal bin Laden.  

"The real benefit to our security from the raid by the Navy Seals is we've recovered a treasure trove of intelligence that can be used to go after bad guys all over the world," said Sen. Tom Carper, a Delaware Democrat and member of the Senate's homeland-security committee. "Our challenge now is to make the most of it and put it to the best use."  

If al Qaeda operatives begin planning retaliatory attacks, their communications could pop them on to the U.S. radar, even if they use couriers to avoid more easily detected electronic communications, officials say.  

U.S. intelligence agencies believe Mr. Zawahiri and other al Qaeda leaders may speed up terror plans in the pipeline to prove al Qaeda's vitality, officials briefed on the matter said.  

Pakistani authorities, meanwhile, now have about 10 of the bin Laden compound's residents in custody and have begun to question them.  

One of the most important leads would be information leading to Mr. Zawahiri, who U.S. officials believe might be on the move as a result of the raid.  

U.S. officials say they believe he is somewhere in Afghanistan or Pakistan. Some intelligence suggests he is hiding in the Pakistani regions of North or South Waziristan, along the Afghanistan border—the tribal region suspected of sheltering bin Laden until investigations led the U.S. to Abbottabad.  

It is too early to know the value of information found in bin Laden's home, and intelligence that initially appears promising sometimes doesn't pan out. U.S. officials were reluctant to describe the data in detail, in part because officials hope the public ambiguity will unnerve al Qaeda members.  

The early assessment from U.S. officials, nonetheless, suggests that in the long run the trove may prove to be a more significant national-security asset than killing bin Laden.  

The Abbottabad strike team went into the bin Laden compound armed with the detailed Sensitive-Site Exploitation plan, which spells out for team members under fire and with limited time which items need to be extracted from a hostile location, and how.  

The plan was rehearsed by team members in advance of the raid. The Seal team was supposed to be inside the compound for no more than 30 minutes, but encountered heavy resistance and had to destroy their disabled Black Hawk helicopter, so the operation lasted about eight minutes longer than planned.  

Team members were assigned specific collection tasks. They carried with them special cases to cart off computers, radios, cellphones, electronic-storage devices such as DVDs, maps, notebooks and books.  

"Think of it like a bank robbery," a senior U.S. official said.  

Raids of residences are usually more valuable than other locations because they turn up personal items the target would have expected to keep private, officials said.  

Officials said bin Laden wasn't found destroying equipment or documents as the strike team closed in. It is unclear if others made an effort to destroy data. "It appears they were more interested in fighting their way out than destroying anything," the official said.  

As the haul is brought back to the U.S., it is being cataloged and processed. U.S. intelligence officers are currently subjecting it to forensic and fingerprint analysis.  

"I think everyone was surprised by the depth and breadth of what he had," a senior administration official said.  

Mike Rogers, who is the chairman of the House Intelligence Committee, said U.S. analysts so far haven't found any "smoking guns" pointing to a specific impending terror plot. But often seemingly small details provide critical pieces to the intelligence puzzle, he said, pointing to the snippet of intelligence—the nickname of one of bin Laden's couriers—that years later led the CIA to his residence.  

Mr. Rogers, a former FBI agent, added that it may be some time before intelligence officials fully understand the scope of the information they have. "There's a lot of hurdles to get over to fully process anything that may come out of a raid," he said.  

Obstacles include language translations, understanding the context of files or documents and verifying the accuracy of certain information.  

When senior al Qaeda leader Abu Zubaydah was captured in 2002, the operation yielded his bank cards, diary, computer disks, notebooks and phone numbers, said Seth Jones, an al Qaeda specialist at Rand Corp. who is writing a book on the terror group.  

That information aided in the capture of other militants, including José Padilla, who was arrested in Chicago that year and later convicted of providing support to terrorists, Mr. Jones said.  

With the death of their leader and his files in U.S. custody, bin Laden's foot soldiers may need to change locations for their own security.  

Once they begin to move, they become easier to detect, although a U.S. intelligence official said there has been as yet "no discernible spike" in communications.  

"I know these individuals now are concerned about their own welfare and well-being. They may be on the move," White House counterterrorism adviser John Brennan told NPR Tuesday.  

Pakistani authorities in Islamabad, the capital, have custody of the four women and six children who survived the firefight, a senior U.S. administration official said. They also have some files and information that the Navy Seals didn't take, he said.  

Pakistani intelligence officials are interrogating bin Laden's 12-year-old daughter, Safia, who saw her father killed by American forces, according to a Pakistani intelligence officer. Safia was with her mother, the official said.  

A U.S. Embassy official in Islamabad said the U.S. hasn't asked Pakistan to hand over bin Laden's family members to American officials.  

Pakistan's foreign office said they would be returned to their country of origin.