Vibrational dynamics of zero-field-splitting hamiltonian in gadolinium-based MRI contrast agents from ab initio molecular dynamics

Journal Article · Mon Jul 07 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4885848· OSTI ID:22308746

Lasoroski, Aurélie ^[1]; Vuilleumier, Rodolphe ^[2]; Pollet, Rodolphe ^[1]

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1. DSM/IRAMIS/NIMBE (CEA-CNRS UMR3299), Commissariat à l’Énergie Atomique, 91191 Gif-sur-Yvette (France)
2. École Normale Supérieure, Département de Chimie, ENS-CNRS-UPMC UMR8640, 75005 Paris (France)

The electronic relaxation of gadolinium complexes used as MRI contrast agents was studied theoretically by following the short time evolution of zero-field-splitting parameters. The statistical analysis of ab initio molecular dynamics trajectories provided a clear separation between static and transient contributions to the zero-field-splitting. For the latter, the correlation time was estimated at approximately 0.1 ps. The influence of the ligand was also probed by replacing one pendant arm of our reference macrocyclic complex by a bulkier phosphonate arm. In contrast to the transient contribution, the static zero-field-splitting was significantly influenced by this substitution.

• OSTI ID: 22308746
• Journal Information: Journal of Chemical Physics, Vol. 141, Issue 1; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
APPROXIMATIONS
CONTRAST MEDIA
GADOLINIUM
GADOLINIUM COMPLEXES
HAMILTONIANS
LIGANDS
MOLECULAR DYNAMICS METHOD
NMR IMAGING