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The key energy scales of Gd-based metallofullerene determined by resonant inelastic X-ray scattering spectroscopy

Shao, Yu-Cheng; Wray, L Andrew; Huang, Shih Wen LU ; Liu, Yi Sheng LU ; Song, Wang; Yang, Shangfeng ; Chuang, Yi-De; Guo, Jinghua and Pong, Way Faung (2017) In Scientific Reports 7(1).
Abstract

Endohedral metallofullerenes, formed by encaging Gd inside fullerenes like C80, can exhibit enhanced proton relaxitivities compared with other Gd-chelates, making them the promising contrast agents for magnetic resonance imaging (MRI). However, the underlying key energy scales of Gd x Sc3-x N@C80 (x = 1-3) remain unclear. Here, we carry out resonant inelastic X-ray scattering (RIXS) experiments on Gd x Sc3-x N@C80 at Gd N 4,5-edges to directly study the electronic structure and spin flip excitations of Gd 4f electrons. Compared with reference Gd2O3 and contrast agent Gadodiamide, the features in the RIXS spectra of all... (More)

Endohedral metallofullerenes, formed by encaging Gd inside fullerenes like C80, can exhibit enhanced proton relaxitivities compared with other Gd-chelates, making them the promising contrast agents for magnetic resonance imaging (MRI). However, the underlying key energy scales of Gd x Sc3-x N@C80 (x = 1-3) remain unclear. Here, we carry out resonant inelastic X-ray scattering (RIXS) experiments on Gd x Sc3-x N@C80 at Gd N 4,5-edges to directly study the electronic structure and spin flip excitations of Gd 4f electrons. Compared with reference Gd2O3 and contrast agent Gadodiamide, the features in the RIXS spectra of all metallofullerenes exhibit broader spectral lineshape and noticeable energy shift. Using atomic multiplet calculations, we have estimated the key energy scales such as the inter-site spin exchange field, intra-atomic 4f-4f Coulomb interactions, and spin-orbit coupling. The implications of these parameters to the 4f states of encapsulated Gd atoms are discussed.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Scientific Reports
volume
7
issue
1
publisher
Nature Publishing Group
external identifiers
  • scopus:85027513213
  • wos:000407570000002
ISSN
2045-2322
DOI
10.1038/s41598-017-08685-5
language
English
LU publication?
yes
id
d67c538e-dd7b-4e78-b7bd-4d2e3c569aa0
date added to LUP
2017-09-05 13:18:59
date last changed
2018-01-07 12:17:58
@article{d67c538e-dd7b-4e78-b7bd-4d2e3c569aa0,
  abstract     = {<p>Endohedral metallofullerenes, formed by encaging Gd inside fullerenes like C<sub>80</sub>, can exhibit enhanced proton relaxitivities compared with other Gd-chelates, making them the promising contrast agents for magnetic resonance imaging (MRI). However, the underlying key energy scales of Gd <sub>x</sub> Sc<sub>3-x</sub> N@C<sub>80</sub> (x = 1-3) remain unclear. Here, we carry out resonant inelastic X-ray scattering (RIXS) experiments on Gd <sub>x</sub> Sc<sub>3-x</sub> N@C<sub>80</sub> at Gd N <sub>4,5</sub>-edges to directly study the electronic structure and spin flip excitations of Gd 4f electrons. Compared with reference Gd<sub>2</sub>O<sub>3</sub> and contrast agent Gadodiamide, the features in the RIXS spectra of all metallofullerenes exhibit broader spectral lineshape and noticeable energy shift. Using atomic multiplet calculations, we have estimated the key energy scales such as the inter-site spin exchange field, intra-atomic 4f-4f Coulomb interactions, and spin-orbit coupling. The implications of these parameters to the 4f states of encapsulated Gd atoms are discussed.</p>},
  articleno    = {8125},
  author       = {Shao, Yu-Cheng and Wray, L Andrew and Huang, Shih Wen and Liu, Yi Sheng and Song, Wang and Yang, Shangfeng  and Chuang, Yi-De and Guo, Jinghua and Pong, Way Faung},
  issn         = {2045-2322},
  language     = {eng},
  month        = {12},
  number       = {1},
  publisher    = {Nature Publishing Group},
  series       = {Scientific Reports},
  title        = {The key energy scales of Gd-based metallofullerene determined by resonant inelastic X-ray scattering spectroscopy},
  url          = {http://dx.doi.org/10.1038/s41598-017-08685-5},
  volume       = {7},
  year         = {2017},
}