Sure.
There were Atheists before Darwin. Long, long before. But I don't think that's really the question posed - did Darwin, by discovering evolution, increase the number of Atheists? In my view, yes, he did. He's not alone in that, all historical science challenges mythical notions of creation; and all current science challenges the need for the supernatural. But Darwin, in explaining humanity, struck a blow to the heart of the need for religion.