Calcium plays an important role in regulating a great variety of neuronal processes, and many efforts are made to generate gadolinium complexes that can act as calcium-dependent MRI contrast agents. A series of gadolinium chelate complexes based on DO3A were developed, bearing phosphonate groups as an additional coordination sites, which is hypothesized to change relaxivity in magnetic resonance experiments dynamically with Ca2+ concentration. Different lengths of the phosphonate side chains are expected to lead to different binding constants of the phosphonate - gadolinium bonds. The latter property can be exploited for fine-tuning the sensitivity of the agent to calcium ion concentration.