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Zinc(II)\u2010dipicolylamine moieties, which are known to bind strongly to phosphates, were introduced in the amide \u201carms\u201d of these ligands, and the interaction of the resulting Gd\u2013Zn<jats:sub>2<\/jats:sub> complexes with a range of anions was screened by using indicator displacement assays (IDAs). Considerable selectivity for polyphosphorylated species (such as pyrophosphate and adenosine\u20105\u2032\u2010triphosphate (ATP)) over a range of other anions (including monophosphorylated anions) was apparent. In addition, we show that pyrophosphate modulates the relaxivity of the gadolinium(III) complex, this modulation being sufficiently large to be observed in imaging experiments. To establish the binding mode of the pyrophosphate and gain insight into the origin of the relaxometric modulation, a series of studies including UV\/Vis and emission spectroscopy, luminescence lifetime measurements in H<jats:sub>2<\/jats:sub>O and D<jats:sub>2<\/jats:sub>O, <jats:sup>17<\/jats:sup>O and <jats:sup>31<\/jats:sup>P\u2005NMR spectroscopy and nuclear magnetic resonance dispersion (NMRD) studies were carried out.<\/jats:p>","DOI":"10.1002\/chem.201001397","type":"journal-article","created":{"date-parts":[[2010,12,7]],"date-time":"2010-12-07T11:45:36Z","timestamp":1291722336000},"page":"223-230","source":"Crossref","is-referenced-by-count":35,"title":["A Pyrophosphate\u2010Responsive Gadolinium(III) MRI Contrast Agent"],"prefix":"10.1002","volume":"17","author":[{"given":"Andrew J.","family":"Surman","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"C\u00e9lia 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