Mr. Pompeo, people familiar with the talks said, suggested that he favored a so-called soft withdrawal, in which Mr. Trump would pull out of the deal but hold off on reimposing some of the sanctions.
On Saturday, the State Department’s chief negotiator, Brian Hook, consulted with European diplomats to try to break a deadlock over the so-called “sunset provisions,” under which the restrictions on Iran’s ability to produce nuclear fuel for civilian use expire after 15 years.
The Europeans had already agreed to a significant compromise: to reimpose sanctions if there was a determination that the Iranians were within 12 months of producing a nuclear weapon. But officials said that still did not satisfy Mr. Trump, and the Europeans were not willing to go any farther.
By Monday, the White House began informing allies that Mr. Trump was going to withdraw from the deal and reimpose oil sanctions and secondary sanctions against the Central Bank of Iran.
Mr. Trump has also instructed the Treasury Department to develop additional sanctions against Iran, a process that could take several weeks.
Under the financial sanctions, European companies will have between 90 days and 180 days to wind down their operations in Iran, or they will run afoul of the American banking system. The oil sanctions will require European and Asian countries to reduce their imports from Iran.
For all the frenzied maneuvering, Mr. Trump seems to have made up his mind several weeks ago. When Mr. Macron visited him two weeks ago, officials said, Mr. Trump told the president that he planned to pull out of the deal on May 12, adding, “I haven’t told Melania yet.”