Magnetic Resonance Imaging (MRI) is rarely used for molecular binding studies and never without synthetic metallic labels. We designed an MRI approach that can selectively detect substrate-target interaction by exploiting the narrow resonance of protons in free substrate for selective radio-frequency (RF) labeling and, subsequently, the process of immobilisation upon binding to a solid-like target for fast dipolar transfer of this label over the protons in its backbone. This cascade of events is ultimately detected via the water MRI signal with enhanced sensitivity. We demonstrate the principle for caffeine binding in vitro and in vivo.
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