skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Pressure-enhanced interplay between lattice, spin, and charge in the mixed perovskite La 2FeMnO 6

Abstract

Spin crossover plays a central role in the structural instability, net magnetic moment modification, metallization, and even in superconductivity in corresponding materials. Most reports on the pressure-induced spin crossover with a large volume collapse have so far focused on compounds with a single transition metal. Here we report a comprehensive high-pressure investigation of a mixed Fe-Mn perovskite La 2FeMnO 6. Under pressure, the strong coupling between Fe and Mn leads to a combined valence/spin transition: Fe 3+(S=5/2) → Fe 2 + (S = 0) and Mn 3+(S = 2) → Mn 4+(S = 3/2), with an isostructural phase transition. The spin transitions of both Fe and Mn are offset by ~20 GPa of the onset pressure, and the lattice collapse occurs in between. Interestingly, Fe 3+ ion shows an abnormal behavior when it reaches a lower valence state (Fe 2+) accompanied by a +0.5 eV energy shift in the Fe K-absorption edge at 15 GPa. This process is associated with the charge-spin-orbital state transition from high spin Fe 3+ to low spin Fe 2+, caused by the significantly enhanced t2g-eg crystal field splitting in the compressed lattice under high pressure. Density functional theory calculations confirm the energy preference of themore » high-pressure state with charge redistribution accompanied by spin state transition of Fe ions. Moreover, La 2FeMnO 6 maintains semiconductor behaviors even when the pressure reached 144.5 GPa as evidenced by the electrical transport measurements, despite the huge resistivity decreasing seven orders of magnitude compared with that at ambient pressure. The investigation carried out here demonstrates high flexibility of double perovskites and their good potentials for optimizing the functionality of these materials.« less

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [4];  [4];  [5];  [5];  [5];  [6];  [1];  [7];  [8];  [2];  [1]
  1. Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
  2. Fudan Univ., Shanghai (China); Nanjing Univ., Nanjing (China)
  3. Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China); Fudan Univ., Shanghai (China)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  6. Chinese Academy of Sciences (CAS), Beijing (China)
  7. Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China); Carnegie Inst. of Washington, Washington, DC (United States). Geophysical Lab.
  8. Univ. zu Köln, Köln (Germany)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1558624
Alternate Identifier(s):
OSTI ID: 1511516
Grant/Contract Number:  
AC02-06CH11357; NA0001974; FG02-99ER45775; FG02-94ER14466; 51527801; U1530402; 11474059; 11674064; 2016YFA0300700
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 99; Journal Issue: 19; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Li, Nana, Fan, Fengren, Sun, Fei, Wang, Yonggang, Zhao, Yongsheng, Liu, Fengliang, Zhang, Qian, Ikuta, Daijo, Xiao, Yuming, Chow, Paul, Heald, Steve M., Sun, Chengjun, Brewe, Dale, Li, Aiguo, Lu, Xujie, Mao, Ho-Kwang, Khomskii, Daniel I., Wu, Hua, and Yang, Wenge. Pressure-enhanced interplay between lattice, spin, and charge in the mixed perovskite La2FeMnO6. United States: N. p., 2019. Web. doi:10.1103/PhysRevB.99.195115.
Li, Nana, Fan, Fengren, Sun, Fei, Wang, Yonggang, Zhao, Yongsheng, Liu, Fengliang, Zhang, Qian, Ikuta, Daijo, Xiao, Yuming, Chow, Paul, Heald, Steve M., Sun, Chengjun, Brewe, Dale, Li, Aiguo, Lu, Xujie, Mao, Ho-Kwang, Khomskii, Daniel I., Wu, Hua, & Yang, Wenge. Pressure-enhanced interplay between lattice, spin, and charge in the mixed perovskite La2FeMnO6. United States. doi:10.1103/PhysRevB.99.195115.
Li, Nana, Fan, Fengren, Sun, Fei, Wang, Yonggang, Zhao, Yongsheng, Liu, Fengliang, Zhang, Qian, Ikuta, Daijo, Xiao, Yuming, Chow, Paul, Heald, Steve M., Sun, Chengjun, Brewe, Dale, Li, Aiguo, Lu, Xujie, Mao, Ho-Kwang, Khomskii, Daniel I., Wu, Hua, and Yang, Wenge. Wed . "Pressure-enhanced interplay between lattice, spin, and charge in the mixed perovskite La2FeMnO6". United States. doi:10.1103/PhysRevB.99.195115.
@article{osti_1558624,
title = {Pressure-enhanced interplay between lattice, spin, and charge in the mixed perovskite La2FeMnO6},
author = {Li, Nana and Fan, Fengren and Sun, Fei and Wang, Yonggang and Zhao, Yongsheng and Liu, Fengliang and Zhang, Qian and Ikuta, Daijo and Xiao, Yuming and Chow, Paul and Heald, Steve M. and Sun, Chengjun and Brewe, Dale and Li, Aiguo and Lu, Xujie and Mao, Ho-Kwang and Khomskii, Daniel I. and Wu, Hua and Yang, Wenge},
abstractNote = {Spin crossover plays a central role in the structural instability, net magnetic moment modification, metallization, and even in superconductivity in corresponding materials. Most reports on the pressure-induced spin crossover with a large volume collapse have so far focused on compounds with a single transition metal. Here we report a comprehensive high-pressure investigation of a mixed Fe-Mn perovskite La2FeMnO6. Under pressure, the strong coupling between Fe and Mn leads to a combined valence/spin transition: Fe3+(S=5/2) → Fe2 + (S = 0) and Mn3+(S = 2) → Mn4+(S = 3/2), with an isostructural phase transition. The spin transitions of both Fe and Mn are offset by ~20 GPa of the onset pressure, and the lattice collapse occurs in between. Interestingly, Fe3+ ion shows an abnormal behavior when it reaches a lower valence state (Fe2+) accompanied by a +0.5 eV energy shift in the Fe K-absorption edge at 15 GPa. This process is associated with the charge-spin-orbital state transition from high spin Fe3+ to low spin Fe2+, caused by the significantly enhanced t2g-eg crystal field splitting in the compressed lattice under high pressure. Density functional theory calculations confirm the energy preference of the high-pressure state with charge redistribution accompanied by spin state transition of Fe ions. Moreover, La2FeMnO6 maintains semiconductor behaviors even when the pressure reached 144.5 GPa as evidenced by the electrical transport measurements, despite the huge resistivity decreasing seven orders of magnitude compared with that at ambient pressure. The investigation carried out here demonstrates high flexibility of double perovskites and their good potentials for optimizing the functionality of these materials.},
doi = {10.1103/PhysRevB.99.195115},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 19,
volume = 99,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 8, 2020
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Epitaxial BiFeO3 Multiferroic Thin Film Heterostructures
journal, March 2003


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996