Ms. Stafford would later use what she learned — in particular the Stanislavski technique — to immerse herself in the world of her subjects, and disappear completely. She moved to New York in 1947 with the dream of making it on Broadway.

It was around this time that she also began experimenting with film. Largely self-taught, her technique was purposefully haphazard, and she used the Russian film pioneer Sergei Eisenstein’s motto to “shoot, shoot, shoot; cut, cut, cut.” She would often work through several rolls of film to home in on her subject and get “the one.”

Though much of her career was carved out through steely determination, Ms. Stafford’s encounter with Einstein was kismet. In 1948, Ms. Stafford, then 24, tagged along with a film crew seeking Einstein’s views on the atomic bomb after Hiroshima. On the drive from Manhattan to the physicist’s home in Princeton, she was handed a 35 millimeter camera and was informed she would be the “stills lady.”

The resulting portrait shows the wizened physicist in a spectral blur — a foggy ghostliness caused by the technical imprecision of a novice, but nevertheless possessing the unmistakable aesthetic that defines a Stafford photograph. After taking the photo, she no longer dreamed of a life before the camera, but, rather, behind it.

In 1949, following an apprenticeship with the New York fashion photographer Francesco Scavullo, Ms. Stafford moved to Paris, where she would spend a decade. There, her love for photography deepened, and she befriended Édith Piaf, Eleanor Roosevelt, Noël Coward and Bing Crosby.

The writer Mulk Raj Anand, her good friend, introduced her to photography greats like Robert Capa and Henri Cartier Bresson, who became her mentors.