Lattice dynamics and elasticity in thermoelectric Mg2Si1-xSnx

Klobes, Benedikt; de Boor, Johannes; Alatas, Ahmet; Hu, Michael Y.; Simon, Ronnie E.; Hermann, Raphaël P.

doi:10.1103/PhysRevMaterials.3.025404

Lattice dynamics and elasticity in thermoelectric ${Mg}_{2} {Si}_{1 - x} {Sn}_{x}$

Journal Article · Thu Feb 28 00:00:00 EST 2019 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.3.025404· OSTI ID:1502500

Klobes, Benedikt ^[1]; de Boor, Johannes ^[2]; Alatas, Ahmet ^[3]; Hu, Michael Y. ^[3]; Simon, Ronnie E. ^[1]; Hermann, Raphaël P. ^[4]

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)

Lattice dynamics and elastic constants in Mg₂Si_1-xSn_x were investigated using resonant ultrasound spectroscopy, Mossbauer spectroscopy, nuclear inelastic scattering, and inelastic x-ray 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 Mg₂Si_1-xSn_x derived from inelastic x-ray 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1502500

Alternate ID(s):: OSTI ID: 1524869
OSTI ID: 1546334

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 2 Vol. 3; ISSN PRMHAR; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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