The Orion capsule will now whip around the Moon, setting the crew up to travel farther from our home planet than any human before.
The astronauts entered what NASA calls the lunar sphere of influence about 0442 GMT Monday and will soon record the first lunar flyby since 1972.
As they entered the Moon's gravitational influence, the crew was about 39,000 miles (63,000 kilometers) from the Moon and about 232,000 miles from Earth, a NASA official said on the agency's livestream of the event.
The historic occasion comes alongside a constellation of firsts for the crew of three Americans and one Canadian. Victor Glover will go down in the books as the first person of color to ever fly around the Moon, and Christina Koch will be the first woman.
Canadian Jeremy Hansen, meanwhile, will become the first non-American to accomplish the feat.
Those three, along with mission commander Reid Wiseman, will spend much of their lunar flyby documenting the Moon.
- 'Far side of the Moon' -
The astronauts have already started seeing features of the celestial body never before viewed with a naked human eye.
In the wee hours of Sunday, NASA published an image taken by the Artemis crew that showed a distant Moon with the Orientale basin visible.
"This mission marks the first time the entire basin has been seen with human eyes," the US space agency said.
The massive crater, which resembles a bullseye, had been photographed before by orbiting cameras.
Koch, speaking to Canadian children live from space, said the crew was most excited to see the basin -- sometimes known as the Moon's "Grand Canyon."
"It's very distinctive and no human eyes previously had seen this crater until today, really, when we were privileged enough to see it," Koch said during the question-and-answer session hosted by the Canadian Space Agency.
Near the end of their flyby, the astronauts will witness a solar eclipse, when the Sun will be behind the Moon and hidden from view aside from its outermost atmosphere, the solar corona.
The four astronauts will also spend some time testing their "Orion crew survival system" spacesuits.
The orange suits protect the crewmembers during launch and reentry, but are also available for emergency use -- they can provide up to six days of breathable air.
The astronauts are the first to ever wear the OCSS suits in space, and will test their functions, including how quickly they can put them on and pressurize them.
While the four astronauts will not touch down on the lunar surface, they are expected to break the record for the farthest distance from Earth during their pass around the Moon.
Over the next day, "they will be on the far side of the Moon, they will eclipse that record, and we're going to learn an awful lot about the spacecraft," NASA administrator Jared Isaacman said Sunday during a televised interview with CNN.
The information will be "pretty paramount to set up for subsequent missions like Artemis 3 in 2027 and, of course, the lunar landing itself on Artemis 4 in 2028," he added.
NASA said the Artemis crew has completed a manual piloting demonstration and reviewed their lunar flyby plan, including reviewing the surface features they must analyze and photograph during their time circling the Moon.
"We're focusing very much on the ecosystem, the life support system of the spacecraft," Isaacman told CNN.
"This is the first time astronauts have ever flown on this spacecraft before," he said. "That's what we're most interested in getting data from."
Here's what you need to know about the event:
NASA will broadcast the flyby live on its website, as well as on YouTube, Amazon and Netflix, with commentary from both the astronauts aboard the mission and experts at the Mission Control center in Houston, Texas.
Given the lengthy distance -- further than any humans have ever traveled from Earth -- NASA has cautioned that the livestream video quality may be poor at times.
"It'll be exciting, you know, in a slightly scary way, when they go behind the moon," Derek Buzasi, a professor of astronomy and astrophysics at the University of Chicago, told AFP.
The academic recalled during the Apollo missions to the Moon, "we all held our breaths a little bit."
Until now, only the Apollo-era astronauts, all of whom were white American men, reached the Moon, between 1968 and 1972.
Shortly before the start of the flyby, the Artemis 2 crew will also reach the furthest distance humans have ever traveled from Earth.
The spacecraft is expected to surpass the Apollo 13 distance record by 4,102 miles (6,600 kilometers) and will reach a maximum distance from the planet of 252,757 miles (406,772 kilometers).
The spaceship will actually swing around the Moon without entering its orbit by following a carefully planned trajectory.
The distance from the Moon will allow astronauts on board to see the complete, circular surface of the Moon, including regions near both poles.
The Moon will appear to the astronauts "about the size of a basketball held at arm's length," Noah Petro, head of NASA's planetary geology lab, told AFP.
The astronauts of the Apollo mission also flew behind the Moon, but they were too close to witness it in entirety.
The Artemis 2 crew will therefore be able to see regions of the Moon that had previously only been captured by robotic imagers.
The four astronauts have gone through years of training to observe and describe the geological formations they observe as accurately as possible.
NASA scientists hope the observations recorded by the crew will provide information about the composition of the Moon and its history, as well as the wider solar system by extension.
For about 53 minutes, their spacecraft will perfectly align with the Moon and the Sun, causing the star to disappear from view.
The astronauts will then have the chance to study the solar corona, the outermost layer of the Sun's atmosphere, which will become visible as a sort of glowing halo.
They will also be on the lookout for possible flashes of light caused by meteorites crashing into the surface of the Moon.
Their position will potentially allow them to recreate the famous "Earthrise" photograph from the Apollo 8 mission in 1968.
The iconic photograph taken by astronaut William Anders captured the bright blue Earth against the vast darkness of space, with the Moon's cratered surface in the foreground.
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