______, Tran, Maya, and their four children left much behind, including their family restaurant. (From ACT test)
Why I can't fill the blank with "after immigrating", but have to be "as immigrants"?
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You are saying "After they arrived they left things behind." They didn't. They left things behind when they departed [from their country].
Saying "As immigrants" only solves the problem if you change the tense of the verb 'leave':
"As immigrants they had left things behind."
It might be clearer to say:
"When they emigrated, Tran, Maya, and their four children left much behind..."
[Btw, immigrate is an AmE word, not a BrE one. If you're not in the US that might be another problem.]