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BERLIN — The diplomatic fallout from the documents harvested by the former NSA contractor Edward J. Snowden intensified Wednesday, with one of the United States’ closest allies, Germany, announcing that its leader had angrily called President Barack Obama, seeking reassurance that her cellphone was not the target of a U.S. intelligence tap.

Washington hastily pledged that Chancellor Angela Merkel, leader of Europe’s most powerful economy, was not the target of current surveillance, and would not be in the future, while conspicuously saying nothing about the past. After a similar furor with France, the call was the second time in 48 hours that the president found himself on the phone with a close European ally to argue that the unceasing revelations of invasive U.S. intelligence gathering should not undermine decades of hard-won trans-Atlantic trust.

Both episodes illustrated the diplomatic challenge to the United States posed by the cache of documents that Snowden handed to the journalist Glenn Greenwald. Last week, Greenwald concluded a deal with the eBay founder Pierre Omidyar to build a new media platform that aims in part to publicize other revelations from the data Greenwald now possesses.

The damage to core U.S. relationships continues to mount. Last month, President Dilma Rousseff of Brazil postponed a state visit to the United States after Brazilian news media reports — fed by material from Greenwald — that the National Security Agency had intercepted messages from Rousseff, her aides and the state oil company, Petrobras. Last weekend, the German newsmagazine Der Spiegel, which has said it has a stack of Snowden documents, suggested that U.S. intelligence had gained access to communications to and from President Felipe Calderón of Mexico when he was still in office.

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U.S. Secretary of State John F. Kerry had barely landed in France on Monday when the newspaper Le Monde disclosed what it said was the mass surveillance of French citizens, as well as spying on French diplomats. Furious, the French summoned the U.S. ambassador, Charles H. Rivkin, and President François Hollande expressed “extreme reprobation” for the reported collection of 70 million phone calls in 30 days late last year and into January.

In a statement published on the website of the national intelligence office Wednesday, James R. Clapper, the director, disputed some aspects of Le Monde’s reporting, calling it misleading and inaccurate in unspecified ways.

He did not address another report by Le Monde that monitoring by the United States had extended to “French diplomatic interests” at the United Nations and in Washington. Information garnered by the NSA played a significant part in a U.N. vote on June 9, 2010, in favor of sanctions against Iran, Le Monde said.

Two senior administration officials — from the State Department and the National Security Council — had arrived in Berlin only hours before the German government disclosed Wednesday that it had received unspecified information that Merkel’s cellphone was under surveillance.

If confirmed, that is “completely unacceptable,” said her spokesman, Steffen Seibert. The accusations followed Der Spiegel disclosures in June of widespread U.S. surveillance of German communications, which struck a specially unsettling chord in a country scarred by the surveillance undertaken by Nazi and Communist governments in its past.

Seibert quoted the chancellor, who was raised in Communist East Germany, as telling Obama that “between close friends and partners, which the Federal Republic of Germany and the United States of America have been for decades, there should be no such surveillance of the communications of a head of government.”

“That would be a grave breach of trust,” Seibert quoted her as saying. “Such practices must cease immediately.”

The government statement did not disclose the source or nature of its suspicions. But Der Spiegel said on its website that Merkel acted after it submitted a reporting inquiry to the government. “Apparently, after an examination by the Federal Intelligence Service and the Federal Office for Security in Information Technology, the government found sufficient plausible grounds to confront the U.S. government,” Der Spiegel wrote.

ARD, Germany’s premier state television channel, said without naming its sources that the supposed monitoring had targeted the Merkel’s official cellphone, not her private one.

About an hour after the news broke in Berlin, Jay Carney, the White House spokesman, appeared before news media in Washington, reporting the Obama-Merkel phone call and saying that “the president assured the chancellor that the United States is not monitoring, and will not monitor, the communications of the chancellor.”

Obama pledged, as he had to Hollande, and to Mexico and Brazil, that intelligence operations were under scrutiny, and that he was aware of the need to balance security against privacy.

The first disclosures from Der Spiegel in June almost soured the long-planned meeting between Obama and Merkel in her capital, which the president visited as a candidate in 2008, delivering a speech before an estimated 200,000 people.

In June, there were far fewer, carefully screened and invited Germans and Americans on hand to hear Obama at the Brandenburg Gate, the symbol of Berlin’s unity and freedom since the Berlin Wall fell in 1989.

Shortly beforehand, Obama and Merkel stood side by side in her chancellery, fielding questions about U.S. surveillance of foreigners’ phone and email traffic. Pressed personally by Merkel, the president said that terrorist threats in Germany were among those foiled by intelligence operations around the world, and Merkel concurred.

Senior intelligence officials have since made plain that cooperation between the United States and Germany in the field is essential to tracking what they view as potential terrorist threats.

But if indeed U.S. intelligence was listening to Merkel’s phone, or registering calls made and received, the trust between Berlin and Washington could be severely damaged. Since June, even senior officials in the German government have voiced more caution about cooperating with the United States, and wondered in private about the extent to which any information gleaned was shared with, say, business rivals of German companies.

The German government said it had been assured that German laws were not broken, but the issue remains politically fragile.

In July, Merkel joked with television interviewers asking about the affair that “I know of no case where I was listened to.”

At a separate news conference that month, she signaled on a more serious note that she understood the importance — for all Western allies — of collecting intelligence. But she also emphasized that German or European laws should not be violated.

The alarm of Americans — and indeed their allies — after the attacks of Sept. 11, 2001, was understandable, Merkel said then, but “the aim does not justify the means. Not everything which is technically doable should be done. The question of relative means must always be answered: What relation is there between the danger and the means we choose, also and especially with regard to preserving the basic rights contained in our Basic Law?”

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