Lattice dynamics and elasticity in thermoelectric ${\mathrm{Mg}}_{2}{\mathrm{Si}}_{1x}{\mathrm{Sn}}_{x}$
Abstract
Lattice dynamics and elastic constants in Mg _{2}Si _{1x}Sn _{x} were investigated using resonant ultrasound spectroscopy, Mossbauer spectroscopy, nuclear inelastic scattering, and inelastic xray scattering. Increasing the Sn content x results in smaller elastic constants, lower Sn specific Debye temperature, lower speed of sound, and a softening of acoustic Sn specific phonons. However, close to band convergence at about x = 0.6, the shear modulus is well below the expected value, which suggests a pronounced connection between band convergence and lattice dynamics in this system. Based on the determined speed of sound and average phonon group velocity, the importance of optical phonons for lattice thermal conductivity is discussed, as the significant reduction in both velocities would yield an implausibly low lattice thermal conductivity of only about 60% of the experimental value. Sn specific thermodynamic quantities calculated from the Sn specific density of phonon states substantiate the general softening of lattice vibrations upon substitution of Si by Sn. A major contribution to the vibrational entropy is thus due to Sn specific vibrational modes. The generalized density of phonon states in Mg _{2}Si _{1x}Sn _{x} derived from inelastic xray scattering for one composition shows that vibrational modes related to lightweight Mg andmore »
 Authors:

 Julich Research Centre (Germany). Julich Centre for Neutron Science (JCNS)
 German Aerospace Center, Koln (Germany)
 Argonne National Lab. (ANL), Argonne, IL (United States)
 Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
 Publication Date:
 Research Org.:
 Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
 Sponsoring Org.:
 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC22)
 OSTI Identifier:
 1502500
 Alternate Identifier(s):
 OSTI ID: 1524869; OSTI ID: 1546334
 Grant/Contract Number:
 AC0206CH11357; AC0500OR22725
 Resource Type:
 Journal Article: Accepted Manuscript
 Journal Name:
 Physical Review Materials
 Additional Journal Information:
 Journal Volume: 3; Journal Issue: 2; Journal ID: ISSN 24759953
 Publisher:
 American Physical Society (APS)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 36 MATERIALS SCIENCE
Citation Formats
Klobes, Benedikt, de Boor, Johannes, Alatas, Ahmet, Hu, Michael Y., Simon, Ronnie E., and Hermann, Raphaël P. Lattice dynamics and elasticity in thermoelectric Mg2Si1xSnx. United States: N. p., 2019.
Web. doi:10.1103/PhysRevMaterials.3.025404.
Klobes, Benedikt, de Boor, Johannes, Alatas, Ahmet, Hu, Michael Y., Simon, Ronnie E., & Hermann, Raphaël P. Lattice dynamics and elasticity in thermoelectric Mg2Si1xSnx. United States. doi:10.1103/PhysRevMaterials.3.025404.
Klobes, Benedikt, de Boor, Johannes, Alatas, Ahmet, Hu, Michael Y., Simon, Ronnie E., and Hermann, Raphaël P. Thu .
"Lattice dynamics and elasticity in thermoelectric Mg2Si1xSnx". United States. doi:10.1103/PhysRevMaterials.3.025404. https://www.osti.gov/servlets/purl/1502500.
@article{osti_1502500,
title = {Lattice dynamics and elasticity in thermoelectric Mg2Si1xSnx},
author = {Klobes, Benedikt and de Boor, Johannes and Alatas, Ahmet and Hu, Michael Y. and Simon, Ronnie E. and Hermann, Raphaël P.},
abstractNote = {Lattice dynamics and elastic constants in Mg2Si1xSnx were investigated using resonant ultrasound spectroscopy, Mossbauer spectroscopy, nuclear inelastic scattering, and inelastic xray scattering. Increasing the Sn content x results in smaller elastic constants, lower Sn specific Debye temperature, lower speed of sound, and a softening of acoustic Sn specific phonons. However, close to band convergence at about x = 0.6, the shear modulus is well below the expected value, which suggests a pronounced connection between band convergence and lattice dynamics in this system. Based on the determined speed of sound and average phonon group velocity, the importance of optical phonons for lattice thermal conductivity is discussed, as the significant reduction in both velocities would yield an implausibly low lattice thermal conductivity of only about 60% of the experimental value. Sn specific thermodynamic quantities calculated from the Sn specific density of phonon states substantiate the general softening of lattice vibrations upon substitution of Si by Sn. A major contribution to the vibrational entropy is thus due to Sn specific vibrational modes. The generalized density of phonon states in Mg2Si1xSnx derived from inelastic xray scattering for one composition shows that vibrational modes related to lightweight Mg and Si set in above 12.5 meV, whereas Sn specific modes are concentrated around 11 meV.},
doi = {10.1103/PhysRevMaterials.3.025404},
journal = {Physical Review Materials},
issn = {24759953},
number = 2,
volume = 3,
place = {United States},
year = {2019},
month = {2}
}
Web of Science
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