Nucera, AlessandroPlatas-Iglesias, CarlosCarniato, FabioBotta, Mauro2024-10-242024-10-242023-11-09Dalton Trans., 2023, 52, 172291477-9234http://hdl.handle.net/2183/39775[Abstract]: We present a detailed relaxometric and computational investigation of three Gd(III) complexes that exist in solution as an equilibrium of two species with a different number of coordinated water molecules: [Gd(H2O)q]3+ (q = 8, 9), [Gd(EDTA)(H2O)q]− and [Gd(CDTA)(H2O)q]− (q = 2, 3). 1H nuclear magnetic relaxation dispersion (NMRD) data were recorded from aqueous solutions of these complexes using a wide Larmor frequency range (0.01–500 MHz). These data were complemented with 17O transverse relaxation rates and chemical shifts recorded at different temperatures. The simultaneous fit of the NMRD and 17O NMR data was guided by computational studies performed at the DFT and CASSCF/NEVPT2 levels, which provided information on Gd⋯H dis-tances, 17O hyperfine coupling constants and the zero-field splitting (ZFS) energy, which affects electronic relaxation. The hydration equilibrium did not have a very im-portant effect in the fits of the experimental data for [Gd(H2O)q]3+ and [Gd(CDTA)(H2O)q]−.engAtribución 3.0 EspañaThis journal is © The Royal Society of Chemistry 2023. This Open Access Article is licensed under a Creative Commons Attribution 3.0 Unported Licence (http://creativecommons.org/licenses/by/3.0/)http://creativecommons.org/licenses/by/3.0/es/Gd(III) complexesEquilibrium speciesCoordinated water moleculesNMRD (Nuclear magnetic relaxation dispersion)Coordination chemistryStructure-dynamics relationshipComputational investigationHydration equilibriaLarmor frequenciesRelaxometric propertiesTransverse relaxation ratejournal articleopen access10.1039/D3DT03413E