Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 8, Pages 4259-4265Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202013923
Keywords
bonding hierarchy; local structure; low phonon modes; rattling dynamics; ultralow lattice thermal conductivity
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Funding
- SERB [CRG/2019/001306]
- Swarnajayanti fellowship (SERB, DST)
- Sheik Saqr fellowship (SSL, ICMS)
- University Grants Commission (UGC)
- DST [RB1868000]
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In this study, lattice dynamics in the Zintl compound TlInTe2 were investigated, revealing that the intrinsic rattling nature of Tl leads to strong phonon scattering and a remarkably low phonon lifetime, resulting in an ultralow thermal conductivity in TlInTe2.
Here, we present lattice dynamics associated with the local chemical bonding hierarchy in Zintl compound TlInTe2, which cause intriguing phonon excitations and strongly suppress the lattice thermal conductivity to an ultralow value (0.46-0.31 W m(-1) K-1) in the 300-673 K. We established an intrinsic rattling nature in TlInTe2 by studying the local structure and phonon vibrations using synchrotron X-ray pair distribution function (PDF) (100-503 K) and inelastic neutron scattering (INS) (5-450 K), respectively. We showed that while 1D chain of covalently bonded InTe2n-n transport heat with Debye type phonon excitation, ionically bonded Tl rattles with a frequency ca. 30 cm(-1) inside distorted Thompson cage formed by InTe2n-n . This highly anharmonic Tl rattling causes strong phonon scattering and consequently phonon lifetime reduces to ultralow value of ca. 0.66(6) ps, resulting in ultralow thermal conductivity in TlInTe2.
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