n- to p-Type Conductivity Transition of Lu<sub>3</sub>N@C<sub>80</sub> Due to Anisotropic Deformation of Fullerene and Pyramidalization of Endohedral Clusters
The endohedral fullerene Lu<sub>3</sub>N@C<sub>80</sub> was examined using in situ high-pressure measurements, which included electrical transport, Fourier-transform infrared spectroscopy, and Raman spectroscopy, in combination with theoretical calculations. Lu<sub>3</sub>N@C<sub>80</sub> was found to undergo a reversible n- to p-type conversion at ∼8.9 GPa. This p-type semiconductor remains stable up to 25 GPa. The fullerene cage collapses at ∼29 GPa, resulting in an irreversible p- to n-type conversion. Raman, infrared, and X-ray absorption spectroscopy reveal that an anisotropic distortion of the carbon cage and a pyramidalization of the planar Lu<sub>3</sub>N clusters occur during compression. Density functional theory simulations indicate that the p orbitals of C atoms in the fullerene cage primarily contribute to the density of states (DOS). Pressure-induced deformation of the fullerene cage dominates the DOS changes in the conduction and valence bands close to the Fermi level. The findings elucidate the relationship between the conductivity and structural changes in the endohedral clusters.
Authors
- Yongjun Tian (ORCID: https://orcid.org/0000-0003-2798-0638)
- Cuiying Pei (ORCID: https://orcid.org/0000-0002-2007-6331)
- Bertil Sundqvist (ORCID: https://orcid.org/0000-0003-0462-6206)
- Zhen Yao (ORCID: https://orcid.org/0000-0001-8325-9832)
- Yaofeng Wang (ORCID: https://orcid.org/0000-0001-5554-8661)
- Zhipeng Yan (ORCID: https://orcid.org/0000-0002-6398-9309)
- Guangtao Liu (ORCID: https://orcid.org/0000-0003-2332-115X)
- Hong Xiao (ORCID: https://orcid.org/0000-0001-8859-9967)
- Sudeshna Samanta (ORCID: https://orcid.org/0000-0001-7341-3808)
- Lin Wang (ORCID: https://orcid.org/0000-0003-2931-7629)
- Ning Chen (ORCID: https://orcid.org/0000-0002-9405-6229)
- Yanpeng Qi (ORCID: https://orcid.org/0000-0003-2722-1375)
Institutions
- Jilin University (CN)
- ShanghaiTech University (CN)
- Soochow University (CN)
- Yanshan University (CN)
- Integrated Optoelectronics (Norway) (NO)
- Jilin Medical University (CN)
- Center for High Pressure Science and Technology Advanced Research (CN)
- V. Bakul Institute for Superhard Materials (UA)
- State Key Laboratory of Metastable Materials Science and Technology
- Umeå University (SE)
Publication Details
- Journal
- Nano Letters
- Published
- 2024-12-06
- DOI
- https://doi.org/10.1021/acs.nanolett.4c04824
- Citations
- 1
- Primary Topic
- Fullerene Chemistry and Applications
- Type
- article
- Field-Weighted Citation Impact
- 0.25
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- Science Challenge Project
- National Safety Academic Fund