John R. Bolton’s political committee, The John Bolton Super PAC, first hired Cambridge in August 2014, months after the firm was founded and while it was still harvesting Facebook data.

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WASHINGTON — The political-action committee founded by John R. Bolton, President Donald Trump’s incoming national-security adviser, was one of the earliest customers of Cambridge Analytica, which it hired specifically to develop psychological profiles of voters with data harvested from tens of millions of Facebook profiles, according to former Cambridge employees and company documents.

Bolton’s political committee, known as The John Bolton Super PAC, first hired Cambridge in August 2014, months after the political-data firm was founded and while it was still harvesting the Facebook data.

In the two years that followed, Bolton’s super PAC spent nearly $1.2 million primarily for “survey research,” which is a term campaigns use for polling, according to campaign-finance records.

But the contract between the committee and Cambridge, a copy of which was obtained by The New York Times, offers more detail on what Bolton was buying. The contract broadly describes the services to be delivered by Cambridge as “behavioral microtargeting with psychographic messaging.”

To do that work, Cambridge used Facebook data, according to the documents and two former employees familiar with the work.

“The data and modeling Bolton’s PAC received was derived from the Facebook data,” said Christopher Wylie, a data expert who was part of the team that founded Cambridge Analytica. “We definitely told them about how we were doing it. We talked about it in conference calls, in meetings.”

Cambridge Analytica, which rose to prominence through its work with Trump’s 2016 election campaign, has found itself confronting a deepening crisis since reports last weekend in The New York Times and The Observer of London that the firm had harvested the data from more than 50 million Facebook profiles in its bid to develop techniques for predicting the behavior of individual U.S. voters.

Cambridge’s so-called psychographic modeling techniques, which were built in part with the data harvested from Facebook, underpinned its work for Trump’s campaign in 2016, setting off a furious — and still unsettled — debate about whether the firm’s technology worked. The same techniques were also the focus of its work for Bolton’s super PAC.

“The Bolton PAC was obsessed with how America was becoming limp-wristed and spineless and it wanted research and messaging for national-security issues,” Wylie said. “That really meant making people more militaristic in their worldview,” he added. “That’s what they said they wanted, anyway.”

Using the psychographic models, Cambridge helped design concepts for advertisements for candidates supported by Bolton’s PAC, including the 2014 campaign of Sen. Thom Tillis, R-N.C., according to Wylie and another former employee, who spoke on condition of anonymity to avoid being dragged into the investigations that now appear to be engulfing Cambridge.

One advertisement, a video posted on YouTube, was aimed at people who scored high for conscientiousness, and were thought to respect hard work and experience. It emphasized Bolton’s time working for Ronald Reagan and how Tillis embodied the spirit and political ethos of the late president.

Beyond their conservative politics, Trump, Bolton and Cambridge Analytica all share a patron: the Mercer family of Long Island, New York, whose patriarch, Robert Mercer, made a fortune at the helm of a top-yielding hedge fund.

Cambridge Analytica, which grew out of the London-based SCL Group, was founded in 2014 with a $15 million investment from Mercer, whose daughter Rebekah sits on the firm’s board of directors. Stephen K. Bannon was also a co-founder.

At this same time, Robert Mercer was financially supporting Bolton’s PAC, donating $5 million between April 2014 and September 2016, according to Federal Election Commission filings. The Mercers also backed Trump in the presidential election.

The Mercer family has not publicly commented since the reports about the misuse of Facebook data by Cambridge first surfaced.

The reports have prompted calls from lawmakers in Britain and the United States for renewed scrutiny of Facebook, and at least two U.S. state prosecutors have said they are looking into the misuse of data by Cambridge Analytica.

The company also suspended its chief executive, Alexander Nix, after a television broadcast this week in which he was recorded suggesting that the company had used seduction and bribery to entrap politicians and influence foreign elections.