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Title: Direct Detection of Dimer Orbitals in Ba 5 AlIr 2 O 11

Abstract

The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous "$${J}_{\mathrm{eff}}=1/2$$ state." Although orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. We directly detect and quantify the formation of dimer orbitals in an iridate material $${\mathrm{Ba}}_{5}{\mathrm{AlIr}}_{2}{\mathrm{O}}_{11}$$ using resonant inelastic x-ray scattering. Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory calculations and theoretical simulations based on an Ir-Ir cluster model. Such partially delocalized dimer states lead to a redefinition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to predictions based on atomic states. This study opens new directions to study dimerization in a large family of materials, including solids, heterostructures, molecules, and transient states.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [5];  [1];  [6]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Condensed Matter Physics and Materials Science
  2. ShanghaiTech Univ. (China). School of Physical Science and Technology; Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics; Univ. of Chinese Academy of Sciences, Beijing (China). School of Physical Sciences
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
  4. Univ. of Colorado, Boulder, CO (United States). Dept. of Physics
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Condensed Matter Physics and Materials Science; Rutgers Univ., Piscataway, NJ (United States). Physics and Astronomy Dept.
  6. ShanghaiTech Univ. (China). School of Physical Science and Technology
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Colorado, Boulder, CO (United States); ShanghaiTech Univ. (China); Chinese Academy of Sciences (CAS), Beijing (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Ministry of Science and Technology (MOST) (China); Chinese Academy of Sciences (CAS) (China); Ministry of Science and Technology of the Republic of China (MOST); Chinese Academy of Sciences (CAS)
OSTI Identifier:
1501559
Alternate Identifier(s):
OSTI ID: 1515549; OSTI ID: 1546180
Report Number(s):
BNL-211400-2019-JAAM
Journal ID: ISSN 0031-9007
Grant/Contract Number:  
SC0012704; AC02-06CH11357; DMR-1712101; 2016YFA0401000; 112111KYSB20170059; 1047478; AC-02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 122; Journal Issue: 10; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electronic structure; magnetism; resonant inelastic x-ray scattering

Citation Formats

Wang, Y., Wang, Ruitang, Kim, Jungho, Upton, M. H., Casa, D., Gog, T., Cao, G., Kotliar, G., Dean, M. P. M., and Liu, X. Direct Detection of Dimer Orbitals in Ba5AlIr2O11. United States: N. p., 2019. Web. doi:10.1103/PhysRevLett.122.106401.
Wang, Y., Wang, Ruitang, Kim, Jungho, Upton, M. H., Casa, D., Gog, T., Cao, G., Kotliar, G., Dean, M. P. M., & Liu, X. Direct Detection of Dimer Orbitals in Ba5AlIr2O11. United States. doi:10.1103/PhysRevLett.122.106401.
Wang, Y., Wang, Ruitang, Kim, Jungho, Upton, M. H., Casa, D., Gog, T., Cao, G., Kotliar, G., Dean, M. P. M., and Liu, X. Mon . "Direct Detection of Dimer Orbitals in Ba5AlIr2O11". United States. doi:10.1103/PhysRevLett.122.106401.
@article{osti_1501559,
title = {Direct Detection of Dimer Orbitals in Ba5AlIr2O11},
author = {Wang, Y. and Wang, Ruitang and Kim, Jungho and Upton, M. H. and Casa, D. and Gog, T. and Cao, G. and Kotliar, G. and Dean, M. P. M. and Liu, X.},
abstractNote = {The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous "${J}_{\mathrm{eff}}=1/2$ state." Although orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. We directly detect and quantify the formation of dimer orbitals in an iridate material ${\mathrm{Ba}}_{5}{\mathrm{AlIr}}_{2}{\mathrm{O}}_{11}$ using resonant inelastic x-ray scattering. Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory calculations and theoretical simulations based on an Ir-Ir cluster model. Such partially delocalized dimer states lead to a redefinition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to predictions based on atomic states. This study opens new directions to study dimerization in a large family of materials, including solids, heterostructures, molecules, and transient states.},
doi = {10.1103/PhysRevLett.122.106401},
journal = {Physical Review Letters},
number = 10,
volume = 122,
place = {United States},
year = {2019},
month = {3}
}

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