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

Title: Heavy-impurity resonance, hybridization, and phonon spectral functions in Fe1-xMxSi, M=Ir,Os

Abstract

The vibrational behavior of heavy substitutional impurities (M=Ir,Os) in Fe1-xMxSi (x = 0, 0.02, 0.04, 0.1) was investigated with a combination of inelastic neutron scattering (INS), transport measurements, and first-principles simulations. In this paper, our INS measurements on single-crystals mapped the four-dimensional dynamical structure factor, S(Q;E), for several compositions and temperatures. Our results show that both Ir and Os impurities lead to the formation of a weakly dispersive resonance vibrational mode, in the energy range of the acoustic phonon dispersions of the FeSi host. We also show that Ir doping, which introduces free carriers and increases electron-phonon coupling, leads to softened interatomic force-constants compared to doping with Os, which is isoelectronic to Fe. We analyze the phonon S(Q,E) from INS through a Green's function model incorporating the phonon self-energy based on first-principles density functional theory (DFT) simulations. Calculations of the quasiparticle spectral functions in the doped system reveal the hybridization between the resonance and the acoustic phonon modes. Finally, our results demonstrate a strong interaction of the host acoustic dispersions with the resonance mode, likely leading to the large observed suppression in lattice thermal conductivity.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1265677
Alternate Identifier(s):
OSTI ID: 1180388
Grant/Contract Number:  
AC05-00OR22725; SC0001299; FG02-09ER46577; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 91; Journal Issue: 9; 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

Delaire, O., Al-Qasir, Iyad I., May, Andrew F., Sales, Brian C., Niedziela, Jennifer L., Ma, Jie, Matsuda, Masaaki, Abernathy, Douglas L., and Berlijn, Tom. Heavy-impurity resonance, hybridization, and phonon spectral functions in Fe1-xMxSi, M=Ir,Os. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.91.094307.
Delaire, O., Al-Qasir, Iyad I., May, Andrew F., Sales, Brian C., Niedziela, Jennifer L., Ma, Jie, Matsuda, Masaaki, Abernathy, Douglas L., & Berlijn, Tom. Heavy-impurity resonance, hybridization, and phonon spectral functions in Fe1-xMxSi, M=Ir,Os. United States. https://doi.org/10.1103/PhysRevB.91.094307
Delaire, O., Al-Qasir, Iyad I., May, Andrew F., Sales, Brian C., Niedziela, Jennifer L., Ma, Jie, Matsuda, Masaaki, Abernathy, Douglas L., and Berlijn, Tom. 2015. "Heavy-impurity resonance, hybridization, and phonon spectral functions in Fe1-xMxSi, M=Ir,Os". United States. https://doi.org/10.1103/PhysRevB.91.094307. https://www.osti.gov/servlets/purl/1265677.
@article{osti_1265677,
title = {Heavy-impurity resonance, hybridization, and phonon spectral functions in Fe1-xMxSi, M=Ir,Os},
author = {Delaire, O. and Al-Qasir, Iyad I. and May, Andrew F. and Sales, Brian C. and Niedziela, Jennifer L. and Ma, Jie and Matsuda, Masaaki and Abernathy, Douglas L. and Berlijn, Tom},
abstractNote = {The vibrational behavior of heavy substitutional impurities (M=Ir,Os) in Fe1-xMxSi (x = 0, 0.02, 0.04, 0.1) was investigated with a combination of inelastic neutron scattering (INS), transport measurements, and first-principles simulations. In this paper, our INS measurements on single-crystals mapped the four-dimensional dynamical structure factor, S(Q;E), for several compositions and temperatures. Our results show that both Ir and Os impurities lead to the formation of a weakly dispersive resonance vibrational mode, in the energy range of the acoustic phonon dispersions of the FeSi host. We also show that Ir doping, which introduces free carriers and increases electron-phonon coupling, leads to softened interatomic force-constants compared to doping with Os, which is isoelectronic to Fe. We analyze the phonon S(Q,E) from INS through a Green's function model incorporating the phonon self-energy based on first-principles density functional theory (DFT) simulations. Calculations of the quasiparticle spectral functions in the doped system reveal the hybridization between the resonance and the acoustic phonon modes. Finally, our results demonstrate a strong interaction of the host acoustic dispersions with the resonance mode, likely leading to the large observed suppression in lattice thermal conductivity.},
doi = {10.1103/PhysRevB.91.094307},
url = {https://www.osti.gov/biblio/1265677}, journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 9,
volume = 91,
place = {United States},
year = {Tue Mar 31 00:00:00 EDT 2015},
month = {Tue Mar 31 00:00:00 EDT 2015}
}

Journal Article:

Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Complex thermoelectric materials
journal, February 2008


Disorder-induced broadening of transverse acoustic phonons in SixGe1−x mixed crystals
journal, July 2004


Role of Disorder and Anharmonicity in the Thermal Conductivity of Silicon-Germanium Alloys: A First-Principles Study
journal, January 2011


Thermoelectric properties of pure and doped FeMSb (M=V,Nb)
journal, January 2000


Effects of Rh on the thermoelectric performance of the p-type Zr0.5Hf0.5Co1−xRhxSb0.99Sn0.01 half-Heusler alloys
journal, May 2010


Stronger phonon scattering by larger differences in atomic mass and size in p-type half-Heuslers Hf1−xTixCoSb0.8Sn0.2
journal, January 2012


The intrinsic disorder related alloy scattering in ZrNiSn half-Heusler thermoelectric materials
journal, November 2014


Localized vibrational modes in metallic solids
journal, October 1998


Breakdown of phonon glass paradigm in La- and Ce-filled Fe4Sb12 skutterudites
journal, August 2008


Effect of filler mass and binding on thermal conductivity of fully filled skutterudites
journal, November 2010


Isotope scattering of dispersive phonons in Ge
journal, January 1983


The nature of the bonds in the iron silicide, FeSi, and related crystals
journal, September 1948


A new high-pressure phase of FeSi
journal, May 2002


Magnetic, transport, and structural properties of Fe 1 x Ir x Si
journal, September 1994


Thermodynamics of FeSi
journal, February 1995


Use of Functional Integrals in Quantum Mechanics and Field Theory
journal, February 1972


Singlet Semiconductor to Ferromagnetic Metal Transition in FeSi
journal, March 1996


Metal-Insulator Transitions in the Kondo Insulator FeSi and Classic Semiconductors Are Similar
journal, April 1997


Heavy fermion metal–Kondo insulator transition in FeSi 1 x Al x
journal, October 1998


Paramagnetic Excited State of FeSi
journal, August 1967


Band structure and semiconducting properties of FeSi
journal, May 1993


Electronic structure and optical properties of FeSi, a strongly correlated insulator
journal, January 1994


ϵ-FeSi: a material sensitive to thermal disorder
journal, December 1997


Electronic structure and magnetism for <mml:math altimg="si46.gif" overflow="scroll" xmlns:xocs="http://www.elsevier.com/xml/xocs/dtd" xmlns:xs="http://www.w3.org/2001/XMLSchema" xmlns:xsi="http://www.w3.org/2001/XMLSchema-instance" xmlns="http://www.elsevier.com/xml/ja/dtd" xmlns:ja="http://www.elsevier.com/xml/ja/dtd" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:tb="http://www.elsevier.com/xml/common/table/dtd" xmlns:sb="http://www.elsevier.com/xml/common/struct-bib/dtd" xmlns:ce="http://www.elsevier.com/xml/common/dtd" xmlns:xlink="http://www.w3.org/1999/xlink" xmlns:cals="http://www.elsevier.com/xml/common/cals/dtd"><mml:msub><mml:mrow><mml:mi>FeSi</mml:mi></mml:mrow><mml:mrow><mml:mo stretchy="false">(</mml:mo><mml:mn>1</mml:mn><mml:mo>-</mml:mo><mml:mi>x</mml:mi><mml:mo stretchy="false">)</mml:mo></mml:mrow></mml:msub><mml:msub><mml:mrow><mml:mi>Ge</mml:mi></mml:mrow><mml:mrow><mml:mi>x</mml:mi></mml:mrow></mml:msub></mml:math> from supercell calculations
journal, December 2004


Phonon softening and metallization of a narrow-gap semiconductor by thermal disorder
journal, March 2011


Thermoelectric properties of Co-, Ir-, and Os-doped FeSi alloys: Evidence for strong electron-phonon coupling
journal, March 2011


Effects of temperature and pressure on phonons in FeSi 1 x Al x
journal, May 2013


Ultraviolet laser photoemission spectroscopy of FeSi: Observation of a gap opening in density of states
journal, December 2005


Angle-resolved photoemission study of the strongly correlated semiconductor FeSi
journal, May 2008


Electron-phonon interaction and spectral weight transfer in Fe 1 x Co x Si
journal, April 2009


Signatures of electronic correlations in iron silicide
journal, February 2012


Doping a semiconductor to create an unconventional metal
journal, August 2008


Optical Evidence of Anderson-Mott Localization in FeSi
journal, November 1994


Static compression of ε-FeSi and an evaluation of reduced silicon as a deep Earth constituent
journal, February 1995


Static compression of iron-silicon alloys: Implications for silicon in the Earth's core: IRON-SILICON ALLOYS
journal, January 2003


Equation of state and elasticity of FeSi
journal, January 2004


Infrared spectroscopic study of phonons coupled to charge excitations in FeSi
journal, February 1997


Adiabatic Electron-Phonon Interaction and High-Temperature Thermodynamics of A 15 Compounds
journal, September 2008


Electron-phonon interactions and high-temperature thermodynamics of vanadium and its alloys
journal, June 2008


Phonon density of states and heat capacity of La 3 x Te 4
journal, November 2009


Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012


Point Defects in Metals II
book, January 1980


Negative Entropy of Mixing for Vanadium-Platinum Solutions
journal, October 2004


Spurious peaks arising from multiple scattering events involving the sample environment in inelastic neutron scattering
journal, June 2014


Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996


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


Projector augmented-wave method
journal, December 1994


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Generalized Gradient Approximation Made Simple
journal, October 1996


Special points for Brillouin-zone integrations
journal, June 1976


Thermal expansion and crystal structure of FeSi between 4 and 1173 K determined by time-of-flight neutron powder diffraction
journal, March 2002


First-Principles Determination of the Soft Mode in Cubic ZrO 2
journal, May 1997


Ab initio calculation of the phonon dispersion relation: Application to Si
journal, March 1982


First-principles studies of the electronic and dynamical properties of monosilicides MSi (M = Fe, Ru, Os)
journal, February 2009


Force-Constant Changes and the Crystal Impurity Problem
journal, November 1971


Local vibrational densities of states of dilute Fe atoms in Al and Cu metals
journal, May 2000


Unfolding First-Principles Band Structures
journal, May 2010


Phonon dispersions in Ga x Al 1 x As alloys
journal, July 1990


Practical application of zone-folding concepts in tight-binding calculations
journal, March 2005


Electron-Phonon Interaction via Electronic and Lattice Wannier Functions: Superconductivity in Boron-Doped Diamond Reexamined
journal, January 2007


Effective Band Structure of Random Alloys
journal, June 2010


Recovering hidden Bloch character: Unfolding electrons, phonons, and slabs
journal, February 2013


Do Transition-Metal Substitutions Dope Carriers in Iron-Based Superconductors?
journal, May 2012


Works referencing / citing this record:

On the microscopic dynamics of the ‘Einstein solids’ AlV 2 Al 20 and GaV 2 Al 20 , and of YV 2 Al 20 : a benchmark system for ‘rattling’ excitations
journal, January 2015


A practical field guide to thermoelectrics: Fundamentals, synthesis, and characterization
journal, June 2018


Giant electromechanical coupling of relaxor ferroelectrics controlled by polar nanoregion vibrations
journal, September 2016


Electronic transport and phonon properties of maximally disordered alloys: From binaries to high-entropy alloys
journal, September 2018


Systematic Quantum Cluster Typical Medium Method for the Study of Localization in Strongly Disordered Electronic Systems
journal, November 2018


Double-Weyl phonons in transition-metal monosilicides
text, January 2017