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

This content will become publicly available on December 9, 2021

Title: Understanding electronic peculiarities in tetragonal FeSe as local structural symmetry breaking

Abstract

Traditional band theory of perfect crystalline solids often uses as input the structure deduced from diffraction experiments; when modeled by the minimal unit cell this often produces a spatially averaged model. The present study illustrates that this is not always a safe practice unless one examines if the intrinsic bonding mechanism is capable of benefiting from the formation of a distribution of lower symmetry local environments that differ from the macroscopically averaged structure. This can happen either due to positional or to magnetic symmetry breaking. By removing the constraint of a small crystallographic cell, the energy minimization in the density functional theory finds atomic and spin symmetry breaking, not evident in conventional diffraction experiments but being found by local probes such as atomic pair distribution function analysis. Here in this paper we report that large atomic and electronic anomalies in bulk tetragonal FeSe emerge from the existence of distributions of local positional and magnetic moment motifs. The found symmetry-broken motifs obtained by minimization of the internal energy represent what chemical bonding in the tetragonal phase prefers as intrinsic energy lowering (stabilizing) static distortions. This explains observations of band renormalization, predicts orbital order and enhanced nematicity, and provides unprecedented close agreementmore » with spectral function measured by photoemission and local atomic environment revealed by the pair distribution function. While the symmetry-restricted strong correlation approach has been argued previously to be the exclusive theory needed for describing the main peculiarities of FeSe, we show here that the symmetry-broken mean-field approach addresses numerous aspects of the problem, provides intuitive insight into the electronic structure, and opens the door for large-scale mean-field calculations for similar d -electron quantum materials.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2];  [3];  [1]
  1. Univ. of Colorado, Boulder, CO (United States). Renewable & Sustainable Energy Inst.
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1732145
Report Number(s):
BNL-220673-2020-JAAM
Journal ID: ISSN 2469-9950
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 102; Journal Issue: 23; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Wang, Zhi, Zhao, Xin-Gang, Koch, Robert, Billinge, Simon L., and Zunger, Alex. Understanding electronic peculiarities in tetragonal FeSe as local structural symmetry breaking. United States: N. p., 2020. Web. https://doi.org/10.1103/physrevb.102.235121.
Wang, Zhi, Zhao, Xin-Gang, Koch, Robert, Billinge, Simon L., & Zunger, Alex. Understanding electronic peculiarities in tetragonal FeSe as local structural symmetry breaking. United States. https://doi.org/10.1103/physrevb.102.235121
Wang, Zhi, Zhao, Xin-Gang, Koch, Robert, Billinge, Simon L., and Zunger, Alex. Wed . "Understanding electronic peculiarities in tetragonal FeSe as local structural symmetry breaking". United States. https://doi.org/10.1103/physrevb.102.235121.
@article{osti_1732145,
title = {Understanding electronic peculiarities in tetragonal FeSe as local structural symmetry breaking},
author = {Wang, Zhi and Zhao, Xin-Gang and Koch, Robert and Billinge, Simon L. and Zunger, Alex},
abstractNote = {Traditional band theory of perfect crystalline solids often uses as input the structure deduced from diffraction experiments; when modeled by the minimal unit cell this often produces a spatially averaged model. The present study illustrates that this is not always a safe practice unless one examines if the intrinsic bonding mechanism is capable of benefiting from the formation of a distribution of lower symmetry local environments that differ from the macroscopically averaged structure. This can happen either due to positional or to magnetic symmetry breaking. By removing the constraint of a small crystallographic cell, the energy minimization in the density functional theory finds atomic and spin symmetry breaking, not evident in conventional diffraction experiments but being found by local probes such as atomic pair distribution function analysis. Here in this paper we report that large atomic and electronic anomalies in bulk tetragonal FeSe emerge from the existence of distributions of local positional and magnetic moment motifs. The found symmetry-broken motifs obtained by minimization of the internal energy represent what chemical bonding in the tetragonal phase prefers as intrinsic energy lowering (stabilizing) static distortions. This explains observations of band renormalization, predicts orbital order and enhanced nematicity, and provides unprecedented close agreement with spectral function measured by photoemission and local atomic environment revealed by the pair distribution function. While the symmetry-restricted strong correlation approach has been argued previously to be the exclusive theory needed for describing the main peculiarities of FeSe, we show here that the symmetry-broken mean-field approach addresses numerous aspects of the problem, provides intuitive insight into the electronic structure, and opens the door for large-scale mean-field calculations for similar d -electron quantum materials.},
doi = {10.1103/physrevb.102.235121},
journal = {Physical Review B},
number = 23,
volume = 102,
place = {United States},
year = {2020},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on December 9, 2021
Publisher's Version of Record

Save / Share:

Works referenced in this record:

The Reflection of X-rays by Crystals
journal, July 1913

  • Bragg, W. H.; Bragg, W. L.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 88, Issue 605
  • DOI: 10.1098/rspa.1913.0040

Quantitative characterization of short-range orthorhombic fluctuations in FeSe through pair distribution function analysis
journal, July 2019


Anomalous temperature evolution of the electronic structure of FeSe
journal, September 2017


Room temperature local nematicity in FeSe superconductor
journal, July 2019


Electronic properties of random alloys: Special quasirandom structures
journal, November 1990


Photoinduced dynamics of nematic order parameter in FeSe
journal, May 2019


Polymorphous nature of cubic halide perovskites
journal, April 2020


Mott Transition and Suppression of Orbital Fluctuations in Orthorhombic 3 d 1 Perovskites
journal, April 2004


Extracting E versus k effective band structure from supercell calculations on alloys and impurities
journal, February 2012


Determination of the Local Lattice Distortions in the Cu O 2 Plane of L a 1.85 S r 0.15 Cu O 4
journal, April 1996


Spin-Orbit Splitting in Compositionally Disordered Semiconductors
journal, November 1972


Direct observation of spin–orbit coupling in iron-based superconductors
journal, December 2015

  • Borisenko, S. V.; Evtushinsky, D. V.; Liu, Z. -H.
  • Nature Physics, Vol. 12, Issue 4
  • DOI: 10.1038/nphys3594

Emergence of the nematic electronic state in FeSe
journal, April 2015


Atomic-Scale Structure of Random Solid Solutions: Extended X-Ray-Absorption Fine-Structure Study of Ga 1 x In x As
journal, November 1982


�ber die Quantenmechanik der Elektronen in Kristallgittern
journal, July 1929


Electronic structure calculations with dynamical mean-field theory
journal, August 2006


An accurate first-principles treatment of doping-dependent electronic structure of high-temperature cuprate superconductors
journal, March 2018


Local structure of ternary semiconducting random solid solutions: Extended x-ray-absorption fine structure of Cd 1 x Mn x Te
journal, August 1984


Effects of atomic short-range order on the electronic and optical properties of GaAsN, GaInN, and GaInAs alloys
journal, February 1998


Orbital Fluctuations in the Different Phases of LaVO 3 and YVO 3
journal, September 2007


Electronic anisotropies revealed by detwinned angle-resolved photo-emission spectroscopy measurements of FeSe
journal, October 2017

  • Watson, Matthew D.; Haghighirad, Amir A.; Rhodes, Luke C.
  • New Journal of Physics, Vol. 19, Issue 10
  • DOI: 10.1088/1367-2630/aa8a04

Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition
journal, August 2019


Direct Observation of Nodes and Twofold Symmetry in FeSe Superconductor
journal, June 2011


Superconductivity in the PbO-type structure  -FeSe
journal, September 2008

  • Hsu, F. -C.; Luo, J. -Y.; Yeh, K. -W.
  • Proceedings of the National Academy of Sciences, Vol. 105, Issue 38
  • DOI: 10.1073/pnas.0807325105

Polymorphous band structure model of gapping in the antiferromagnetic and paramagnetic phases of the Mott insulators MnO, FeO, CoO, and NiO
journal, January 2018


Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser
journal, July 2017


Ground-state structures and the random-state energy of the Madelung lattice
journal, December 1990


Kinetic frustration and the nature of the magnetic and paramagnetic states in iron pnictides and iron chalcogenides
journal, September 2011

  • Yin, Z. P.; Haule, K.; Kotliar, G.
  • Nature Materials, Vol. 10, Issue 12
  • DOI: 10.1038/nmat3120

Effective Band Structure of Random Alloys
journal, June 2010


Effects of disorder on the vibrational properties of SiGe alloys: Failure of mean-field approximations
journal, September 1992


PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals
journal, July 2007


The classification of tilted octahedra in perovskites
journal, November 1972

  • Glazer, A. M.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 11
  • DOI: 10.1107/S0567740872007976

Short-range-order types in binary alloys: a reflection of coherent phase stability
journal, March 2000


A first-principle perspective on electronic nematicity in FeSe
journal, July 2020


Special quasirandom structures
journal, July 1990


Lifting of xz / yz orbital degeneracy at the structural transition in detwinned FeSe
journal, September 2014


Role of the orbital degree of freedom in iron-based superconductors
journal, October 2017


Neutron scattering measurements of the phonon density of states of FeSe 1 x superconductors
journal, January 2009


Direct Observation of the Formation of Polar Nanoregions in Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3 Using Neutron Pair Distribution Function Analysis
journal, April 2005


What drives nematic order in iron-based superconductors?
journal, January 2014

  • Fernandes, R. M.; Chubukov, A. V.; Schmalian, J.
  • Nature Physics, Vol. 10, Issue 2
  • DOI: 10.1038/nphys2877

A profile refinement method for nuclear and magnetic structures
journal, June 1969


Structurally triggered metal-insulator transition in rare-earth nickelates
journal, November 2017


Symmetry-breaking polymorphous descriptions for correlated materials without interelectronic U
journal, July 2020


Structures and phase transitions in the ordered double perovskites Ba 2 Bi III Bi V O 6 and Ba 2 Bi III Sb V O 6
journal, July 2006

  • Kennedy, Brendan J.; Howard, Christopher J.; Knight, Kevin S.
  • Acta Crystallographica Section B Structural Science, Vol. 62, Issue 4
  • DOI: 10.1107/S0108768106018842

“Majority Representation” of Alloy Electronic States
journal, May 1998


Crystal structure of the new FeSe1−x superconductor
journal, January 2008

  • Margadonna, Serena; Takabayashi, Yasuhiro; McDonald, Martin T.
  • Chemical Communications, Issue 43
  • DOI: 10.1039/b813076k

Theoretical approaches to x-ray absorption fine structure
journal, July 2000


Origin of band gaps in 3d perovskite oxides
journal, April 2019