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Title: Synthesis, crystal chemistry and physical properties of the Ruddlesden-Popper phases Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} (0=<x=<1.0)

Abstract

The crystal chemistry, electronic structure, and electrical and magnetic properties of the novel perovskite-related nickel oxides Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} with 0=<x=<1.0 have been studied. X-ray diffraction and selected area electron diffraction (ED) data indicate that the samples have a tetragonal (Space group I4/mmm) structure. ED patterns and high-resolution images reveal the presence of a regular stacking along the c-axis for the x=1.0 sample. The lattice parameters, oxygen content, and average oxidation state of iron and nickel decrease with increasing Ni content. The electronic structure of the x=1.0 sample was studied by M 2p X-ray photoelectron spectroscopy (XPS). An analysis of the spectra using the cluster model indicates that this material is in the negative charge-transfer regime and the ground state is dominated by the 3d{sup n+1}L configuration with 2p holes (L) in the oxygen band. The insulator states are stabilized due to a p-p type band gap that arises because the p-d transfer integral T{sub {sigma}} dominates over the O 2p bandwith. Although magnetic measurements reveal the presence of ferromagnetic interactions that lead to magnetic frustration at T=<40K, no long-range magnetic order was observed for the samples with x>=0.3. The electrical resistivity decreases with increasing Ni content asmore » the p-p band gap tend to close due to the reduction of the T{sub {sigma}} value. Negative magnetoresistance ({approx}-24% for x=0.6 and -7% for x=1.0 at 20K and 9T) was observed for the Ni containing samples.« less

Authors:
 [1];  [1];  [1];  [2];  [1];  [3];  [1]
  1. Centro Atomico Bariloche, CNEA, Av. E. Bustillo 9500, 8400 San Carlos de Bariloche (Argentina)
  2. Departamento de Fisica, Universidade Federal do Parana, Caixa Postal 19091, 81531-990 Curitiba PR (Brazil)
  3. Materials Science and Engineering Program, University of Texas at Austin, Austin, TX 78712 (United States)
Publication Date:
OSTI Identifier:
20725934
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 178; Journal Issue: 5; Other Information: DOI: 10.1016/j.jssc.2005.02.018; PII: S0022-4596(05)00079-4; Copyright (c) 2005 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CLUSTER MODEL; CRYSTALS; ELECTRON DIFFRACTION; ELECTRONIC STRUCTURE; IRON COMPOUNDS; LATTICE PARAMETERS; MAGNETIC PROPERTIES; MAGNETORESISTANCE; NICKEL OXIDES; PEROVSKITE; SPACE GROUPS; STRONTIUM COMPOUNDS; TETRAGONAL LATTICES; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY

Citation Formats

Mogni, Liliana, Prado, Fernando, Ascolani, Hugo, Abbate, Miguel, Moreno, Mario S, Manthiram, Arumugam, and Caneiro, Alberto. Synthesis, crystal chemistry and physical properties of the Ruddlesden-Popper phases Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} (0=<x=<1.0). United States: N. p., 2005. Web. doi:10.1016/j.jssc.2005.02.018.
Mogni, Liliana, Prado, Fernando, Ascolani, Hugo, Abbate, Miguel, Moreno, Mario S, Manthiram, Arumugam, & Caneiro, Alberto. Synthesis, crystal chemistry and physical properties of the Ruddlesden-Popper phases Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} (0=<x=<1.0). United States. https://doi.org/10.1016/j.jssc.2005.02.018
Mogni, Liliana, Prado, Fernando, Ascolani, Hugo, Abbate, Miguel, Moreno, Mario S, Manthiram, Arumugam, and Caneiro, Alberto. 2005. "Synthesis, crystal chemistry and physical properties of the Ruddlesden-Popper phases Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} (0=<x=<1.0)". United States. https://doi.org/10.1016/j.jssc.2005.02.018.
@article{osti_20725934,
title = {Synthesis, crystal chemistry and physical properties of the Ruddlesden-Popper phases Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} (0=<x=<1.0)},
author = {Mogni, Liliana and Prado, Fernando and Ascolani, Hugo and Abbate, Miguel and Moreno, Mario S and Manthiram, Arumugam and Caneiro, Alberto},
abstractNote = {The crystal chemistry, electronic structure, and electrical and magnetic properties of the novel perovskite-related nickel oxides Sr{sub 3}Fe{sub 2-x}Ni{sub x}O{sub 7-{delta}} with 0=<x=<1.0 have been studied. X-ray diffraction and selected area electron diffraction (ED) data indicate that the samples have a tetragonal (Space group I4/mmm) structure. ED patterns and high-resolution images reveal the presence of a regular stacking along the c-axis for the x=1.0 sample. The lattice parameters, oxygen content, and average oxidation state of iron and nickel decrease with increasing Ni content. The electronic structure of the x=1.0 sample was studied by M 2p X-ray photoelectron spectroscopy (XPS). An analysis of the spectra using the cluster model indicates that this material is in the negative charge-transfer regime and the ground state is dominated by the 3d{sup n+1}L configuration with 2p holes (L) in the oxygen band. The insulator states are stabilized due to a p-p type band gap that arises because the p-d transfer integral T{sub {sigma}} dominates over the O 2p bandwith. Although magnetic measurements reveal the presence of ferromagnetic interactions that lead to magnetic frustration at T=<40K, no long-range magnetic order was observed for the samples with x>=0.3. The electrical resistivity decreases with increasing Ni content as the p-p band gap tend to close due to the reduction of the T{sub {sigma}} value. Negative magnetoresistance ({approx}-24% for x=0.6 and -7% for x=1.0 at 20K and 9T) was observed for the Ni containing samples.},
doi = {10.1016/j.jssc.2005.02.018},
url = {https://www.osti.gov/biblio/20725934}, journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = 5,
volume = 178,
place = {United States},
year = {Sun May 15 00:00:00 EDT 2005},
month = {Sun May 15 00:00:00 EDT 2005}
}