Observation of the origin of d0 magnetism in ZnO nanostructures using X-ray-based microscopic and spectroscopic techniques

Shashi B. Singh, Yu Fu Wang, Yu Cheng Shao, Hsuan Yu Lai, Shang Hsien Hsieh, Mukta V. Limaye, Chen Hao Chuang, Hung Chung Hsueh, Hsaiotsu Wang, Jau Wern Chiou, Hung Ming Tsai, Chih Wen Pao, Chia Hao Chen, Hong Ji Lin, Jyh Fu Lee, Chun Te Wu, Jih Jen Wu, Way Faung Pong, Takuji Ohigashi, Nobuhiro KosugiJian Wang, Jigang Zhou, Tom Regier, Tsun Kong Sham

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44 Citations (Scopus)

Abstract

Efforts have been made to elucidate the origin of d0 magnetism in ZnO nanocactuses (NCs) and nanowires (NWs) using X-ray-based microscopic and spectroscopic techniques. The photoluminescence and O K-edge and Zn L 3,2-edge X-ray-excited optical luminescence spectra showed that ZnO NCs contain more defects than NWs do and that in ZnO NCs, more defects are present at the O sites than at the Zn sites. Specifically, the results of O K-edge scanning transmission X-ray microscopy (STXM) and the corresponding X-ray-absorption near-edge structure (XANES) spectroscopy demonstrated that the impurity (non-stoichiometric) region in ZnO NCs contains a greater defect population than the thick region. The intensity of O K-edge STXM-XANES in the impurity region is more predominant in ZnO NCs than in NWs. The increase in the unoccupied (occupied) density of states at/above (at/below) the conduction-band minimum (valence-band maximum) or the Fermi level is related to the population of defects at the O sites, as revealed by comparing the ZnO NCs to the NWs. The results of O K-edge and Zn L3,2-edge X-ray magnetic circular dichroism demonstrated that the origin of magnetization is attributable to the O 2p orbitals rather than the Zn d orbitals. Further, the local density approximation (LDA) + U verified that vacancies in the form of dangling or unpaired 2p states (due to Zn vacancies) induced a significant local spin moment in the nearest-neighboring O atoms to the defect center, which was determined from the uneven local spin density by analyzing the partial density of states of O 2p in ZnO. This journal is

Original languageEnglish
Pages (from-to)9166-9176
Number of pages11
JournalNanoscale
Volume6
Issue number15
DOIs
Publication statusPublished - 2014 Aug 7

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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