title: Water exchange of a ProHance MRI contrast agent: isomer-dependent free-energy landscapes and mechanisms.
abstract: The water-exchange reaction in two diastereoisomers of the clinical magnetic resonance imaging contrast agent [Gd(HP-DO3A)(H(2)O)] (also known as ProHance) has been studied using ab initio simulations. On the basis of the molecular-level details of the mechanism derived from these simulations in aqueous solution, we unravel the underlying difference in the free energies and mechanisms of water exchange in the two diastereoisomers. These findings reveal the crucial role played by hydrogen-bonding dynamics and thus suggest their appropriate control in tailoring improved gadolinium-based constrast agents.
authors.affiliation: DSM/IRAMIS/SIS2M (CEA-CNRS UMR3299), Commissariat à l'Énergie Atomique, 91191 Gif-sur-Yvette, France. rodolphe.pollet@cea.fr
authors.forename: Rodolphe
authors.initials: R
authors.lastname: Pollet
authors.forename: Nisanth N
authors.initials: NN
authors.lastname: Nair
authors.forename: Dominik
authors.initials: D
authors.lastname: Marx
mesh_terms: D003287:Contrast Media / Q000737:chemistry*; D005682:Gadolinium; D006571:Heterocyclic Compounds / Q000737:chemistry*; D008279:Magnetic Resonance Imaging; D009942:Organometallic Compounds / Q000737:chemistry*; D011789:Quantum Theory; D013237:Stereoisomerism; D014867:Water / Q000737:chemistry*
chemical_list: D003287:Contrast Media; D006571:Heterocyclic Compounds; D009942:Organometallic Compounds; C062402:gadoteridol; D014867:Water; D005682:Gadolinium