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

Journal Article · · Scientific Reports
 [1];  [2];  [3];  [4];  [5];  [5]; ORCiD logo [4]; ORCiD logo [6];  [1]
  1. Tamkang Univ., Taipei (Taiwan). Dept. of Physics
  2. New York Univ. (NYU), NY (United States). Dept. of Physics
  3. Lund Univ. (Sweden). MAX IV Lab.
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Univ. of Science and Technology of China, Hefei (China). Hefei National Lab. for Physical Sciences at Microscale, CAS Key Lab. of Materials for Energy Conversion, Dept. of Materials Science and Engineering, Synergetic Innovation Center of Quantum Information and Quantum Physics
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Santa Cruz, CA (United States). Dept. of Chemistry and Biochemistry
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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-xN@C80 (x = 1–3) remain unclear. Here, we carry out resonant inelastic x-ray scattering (RIXS) experiments on GdxSc3-xN@C80 at Gd N4,5-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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231; NSC 102-2112-M032-007-MY3; NSC 102-2632-M032-001-MY3; DMR-1420073
OSTI ID:
1408489
Journal Information:
Scientific Reports, Vol. 7, Issue 1; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

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