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Metal complexes have increasing importance in modern medicine. Early recognition of diseases, which is the cornerstone of successful therapies, is one of the most important goals in medical imaging. To meet this challenge, one needs to explore and to visualize the alterations in the molecular events of biological processes, from the homeostasis of a simple metal ion to the complex functioning of biomolecular assemblies. For this, even the most sophisticated instrumentational tools like MRI, PET, SPECT or optical imaging need to be complemented with the appropriate chemistry. Many of the diagnostic agents, indispensable in molecular imaging approaches, are based on metal complexes.