Despite being a complex many-body system, the atomic nucleus exhibits simple structures for certain "magic" numbers of protons and neutrons. The calcium chain in particular is both unique and puzzling: evidence of doubly-magic features are known in 40,48Ca, and recently suggested in two radioactive isotopes, 52,54Ca. Although many properties of experimentally known Ca isotopes have been successfully described by nuclear theory, it is still a challenge to predict their charge radii evolution. Here we present the first measurements of the charge radii of 49,51,52Ca, obtained from laser spectroscopy experiments at ISOLDE, CERN. The experimental results are complemented by state-of-the-art theoretical calculations. The large and unexpected increase of the size of the neutron-rich calcium isotopes beyond N = 28 challenges the doubly-magic nature of 52Ca and opens new intriguing questions on the evolution of nuclear sizes away from stability, which are of importance for our understanding of neutron-rich atomic nuclei.