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The word "大都市" is formed by combining three characters: "大" meaning "big" or "large", "都" meaning "capital" or "metropolis", and "市" meaning "city", with "都市" together meaning "city" or "metropolis", so "大" modifies "都市" to specify a large metropolitan area.

Word Definition - 大都市

dà dū shì metropolis; large city; megacity