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

Title: Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates

Abstract

Many-body effects produce deviations from the predictions of conventional band theory in quantum materials, leading to strongly correlated phases with insulating or bad metallic behavior. One example is the rare-earth nickelates RNiO 3, which undergo metal-to-insulator transitions (MITs) whose origin is debated. Here, we combine total neutron scattering and broadband dielectric spectroscopy experiments to study and compare carrier dynamics and local crystal structure in LaNiO 3 and NdNiO 3. We find that the local crystal structure of both materials is distorted in the metallic phase, with slow, thermally activated carrier dynamics at high temperature. We further observe a sharp change in conductivity across the MIT in NdNiO 3, accompanied by slight differences in the carrier hopping time. Here, these results suggest that changes in carrier concentration drive the MIT through a polaronic mechanism, where the (bi)polaron liquid freezes into the insulating phase across the MIT temperature.

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. The Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Instituto de Ciencia de Materiales de Madrid, Madrid (Spain)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1484150
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Shamblin, Jacob, Heres, Maximilian, Zhou, Haidong, Sangoro, Joshua, Lang, Maik, Neuefeind, Joerg, Alonso, J. A., and Johnston, Steven. Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates. United States: N. p., 2018. Web. doi:10.1038/s41467-017-02561-6.
Shamblin, Jacob, Heres, Maximilian, Zhou, Haidong, Sangoro, Joshua, Lang, Maik, Neuefeind, Joerg, Alonso, J. A., & Johnston, Steven. Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates. United States. doi:10.1038/s41467-017-02561-6.
Shamblin, Jacob, Heres, Maximilian, Zhou, Haidong, Sangoro, Joshua, Lang, Maik, Neuefeind, Joerg, Alonso, J. A., and Johnston, Steven. Mon . "Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates". United States. doi:10.1038/s41467-017-02561-6. https://www.osti.gov/servlets/purl/1484150.
@article{osti_1484150,
title = {Experimental evidence for bipolaron condensation as a mechanism for the metal-insulator transition in rare-earth nickelates},
author = {Shamblin, Jacob and Heres, Maximilian and Zhou, Haidong and Sangoro, Joshua and Lang, Maik and Neuefeind, Joerg and Alonso, J. A. and Johnston, Steven},
abstractNote = {Many-body effects produce deviations from the predictions of conventional band theory in quantum materials, leading to strongly correlated phases with insulating or bad metallic behavior. One example is the rare-earth nickelates RNiO3, which undergo metal-to-insulator transitions (MITs) whose origin is debated. Here, we combine total neutron scattering and broadband dielectric spectroscopy experiments to study and compare carrier dynamics and local crystal structure in LaNiO3 and NdNiO3. We find that the local crystal structure of both materials is distorted in the metallic phase, with slow, thermally activated carrier dynamics at high temperature. We further observe a sharp change in conductivity across the MIT in NdNiO3, accompanied by slight differences in the carrier hopping time. Here, these results suggest that changes in carrier concentration drive the MIT through a polaronic mechanism, where the (bi)polaron liquid freezes into the insulating phase across the MIT temperature.},
doi = {10.1038/s41467-017-02561-6},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Charge Disproportionation without Charge Transfer in the Rare-Earth-Element Nickelates as a Possible Mechanism for the Metal-Insulator Transition
journal, March 2014


Dimensionality Control of Electronic Phase Transitions in Nickel-Oxide Superlattices
journal, May 2011


Momentum-Resolved Electronic Structure of the High- T c Superconductor Parent Compound BaBiO 3
journal, July 2016


Band gaps and electronic structure of transition-metal compounds
journal, July 1985


Charge Ordering as Alternative to Jahn-Teller Distortion
journal, April 2007


EXPGUI , a graphical user interface for GSAS
journal, April 2001


Electronic properties of the metallic perovskite LaNiO 3 : Correlated behavior of 3 d electrons
journal, September 1992


On the use of modification functions when Fourier transforming total scattering data
journal, October 2012


Structural, magnetic and electronic properties of perovskites (R = rare earth)
journal, February 1997


Site-Selective Mott Transition in Rare-Earth-Element Nickelates
journal, October 2012


Physics of Ultrathin Films and Heterostructures of Rare-Earth Nickelates
journal, July 2016


Metal-insulator transitions
journal, October 1998

  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/RevModPhys.70.1039

Hall effect measurements on epitaxial SmNiO 3 thin films and implications for antiferromagnetism
journal, March 2013


Electronic structure of PrNiO 3 studied by photoemission and x-ray-absorption spectroscopy: Band gap and orbital ordering
journal, November 1995


Insulating Pockets in Metallic LaNiO 3
journal, November 2015

  • Li, Bing; Louca, Despina; Yano, Shinichiro
  • Advanced Electronic Materials, Vol. 2, Issue 2
  • DOI: 10.1002/aelm.201500261

Polar metals by geometric design
journal, April 2016


The dynamics of charge-density waves
journal, October 1988


The Nanoscale Ordered MAterials Diffractometer NOMAD at the Spallation Neutron Source SNS
journal, September 2012

  • Neuefeind, Jörg; Feygenson, Mikhail; Carruth, John
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 287
  • DOI: 10.1016/j.nimb.2012.05.037

Giant O 16 O 18 Isotope Effect on the Metal-Insulator Transition of R NiO 3 Perovskites ( R = Rare Earth)
journal, March 1998


Systematic study of insulator-metal transitions in perovskites RNiO3 (R=Pr,Nd,Sm,Eu) due to closing of charge-transfer gap
journal, April 1992


Bond disproportionation and dynamical charge fluctuations in the perovskite rare-earth nickelates
journal, November 2016


μSR study of short-range charge order in YNiO3 above the monoclinic–orthorhombic transition
journal, March 2006


Origins of bad-metal conductivity and the insulator–metal transition in the rare-earth nickelates
journal, March 2014

  • Jaramillo, R.; Ha, Sieu D.; Silevitch, D. M.
  • Nature Physics, Vol. 10, Issue 4
  • DOI: 10.1038/nphys2907

Metal-Insulator Transition in Ultrathin LaNiO 3 Films
journal, June 2011


Hybridization effects and bond disproportionation in the bismuth perovskites
journal, March 2015


Orbital reflectometry of oxide heterostructures
journal, February 2011

  • Benckiser, Eva; Haverkort, Maurits W.; Brück, Sebastian
  • Nature Materials, Vol. 10, Issue 3
  • DOI: 10.1038/nmat2958

Short-range charge order in R Ni O 3 perovskites ( R = Pr , Nd, Eu, Y) probed by x-ray-absorption spectroscopy
journal, January 2005

  • Piamonteze, Cínthia; Tolentino, Hélio C. N.; Ramos, Aline Y.
  • Physical Review B, Vol. 71, Issue 1
  • DOI: 10.1103/PhysRevB.71.012104

Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates
journal, October 2016

  • Bisogni, Valentina; Catalano, Sara; Green, Robert J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13017

Tunable Charge and Spin Order in PrNiO 3 Thin Films and Superlattices
journal, November 2014


Origin of the band gap in the negative charge-transfer-energy compound NaCuO 2
journal, September 1991


Probing Nanoscale Ion Dynamics in Ultrathin Films of Polymerized Ionic Liquids by Broadband Dielectric Spectroscopy
journal, August 2016


Theory of the Magnetic and Metal-Insulator Transitions in R NiO 3 Bulk and Layered Structures
journal, March 2013


Charge disproportionation in R NiO 3 perovskites ( R = rare earth) from high-resolution x-ray absorption spectroscopy
journal, December 2009


The random free‐energy barrier model for ac conduction in disordered solids
journal, September 1988

  • Dyre, Jeppe C.
  • Journal of Applied Physics, Vol. 64, Issue 5
  • DOI: 10.1063/1.341681

    Works referencing / citing this record:

    Disentangling lattice and electronic contributions to the metal–insulator transition from bulk vs. layer confined RNiO 3
    journal, July 2019

    • Georgescu, Alexandru B.; Peil, Oleg E.; Disa, Ankit S.
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 29
    • DOI: 10.1073/pnas.1818728116

    Anomalous electron transport in epitaxial NdNiO 3 films
    journal, June 2019