Water-soluble multi-hydroxyl lanthanoid (La, Ce, Gd, Dy, and Er) endohedral metallofullerenes (metallofullerenols, M@C(82)(OH)(n)()) have been synthesized and characterized for the use of magnetic resonance imaging (MRI) contrast agents. The observed longitudinal and transverse relaxivities for water protons, r(1) and r(2), of the metallofullerenols are in the range 0.8-73 and 1.2-80 (sec(-1)mM(-1)), respectively, which are significantly higher than those of the corresponding lanthanoid-DTPA chelate complexes. Among these Gd-metallofullerenols, Gd@C(82)(OH)(n)() has exhibited the highest r(1) and r(2) values in consistent with our previous results. The observed large r(1) of the current metallofullerenols can mainly be ascribed to the dipole-dipole relaxation together with a substantial decrease of the overall molecular rotational motion. The large r(2), except for the Gd-metallofullerenols, have been attributed to the so-called Curie spin relaxation. The MRI phantom studies are also performed and are consistent with these results. The metallofullerenols will be an ideal model for future MRI contrast agents with higher proton relaxivities.
The La2@C72 metallofullerene having the so-called "missing" C72 fullerene cage was structurally elucidated by using 13C NMR and 139La NMR spectroscopy. The obtained structure of La2@C72 does not satisfy fullerene's structural golden rule, that is, the isolated-pentagon rule. The structure is consistent with a non-IPR D2-C72 (#10611) cage structure where each La atom is situated close to one of the two-fused pentagons.
We first demonstrate a field-effect-transistor operation of dimetallofullerene La2@C80 with the icosahedral cage symmetry. The thin-film device showed an n-type behavior with a mobility of 1.1 x 10-4 cm2/V s at room temperature under high vacuum. Taking the nature of LUMO into account, the n-type behavior indicates an occurrence of carrier conduction through encapsulated La ions. The low mobility, suggesting an intermolecular hopping mechanism, is ascribed to the intrinsic and extrinsic reasons, which are discussed in the text.
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