BERLIN — The German government on Thursday demanded the removal of the top American spy in the country, the strongest evidence yet that mounting revelations about widespread American intelligence operations in Germany have gravely damaged relations between once close allies.

The decision by Chancellor Angela Merkel to publicly announce the expulsion of the Central Intelligence Agency’s Berlin station chief was seen as a highly symbolic expression of the deep anger and hurt that German officials have felt since the exposure of the American espionage operations.

It is likely to force another reassessment inside the C.I.A. and other spy agencies about whether provocative espionage operations in friendly nations are worth the risk to broader foreign policy goals. One such assessment was conducted last summer, when President Obama ordered a halt to the tapping of Ms. Merkel’s phone after it came to light because of the former National Security Agency contractor Edward J. Snowden.

Current and former American officials said that the Berlin station chief, who works undercover, has been in the position for about a year. It was his predecessor in the job, the officials said, who oversaw the recruitment of the German intelligence officer arrested last week who has reportedly told his interrogators he was spying for the C.I.A., touching off a storm of criticism of the United States. German investigators are also looking at a second case of an official inside the Defense Ministry who may have been working for the Americans.