journal article·2013-06Open access

Glass-like phonon scattering from a spontaneous nanostructure in AgSbTe2

J. Ma, O. Delaire, A. F. May, C. E. Carlton, M. A. McGuire, L. H. VanBebber, D. L. Abernathy, G. Ehlers, Tao Hong, A. Huq, Wei Tian, V. M. Keppens, Y. Shao-Horn, B. C. Sales

Nature Nanotechnology· Volume 8· Issue 6

Abstract

Materials with very low thermal conductivity are of great interest for both thermoelectric and optical phase-change applications. Synthetic nanostructuring is most promising for suppressing thermal conductivity through phonon scattering, but challenges remain in producing bulk samples. In crystalline AgSbTe2 we show that a spontaneously forming nanostructure leads to a suppression of thermal conductivity to a glass-like level. Our mapping of the phonon mean free paths provides a novel bottom-up microscopic account of thermal conductivity and also reveals intrinsic anisotropies associated with the nanostructure. Ground-state degeneracy in AgSbTe2 leads to the natural formation of nanoscale domains with different orderings on the cation sublattice, and correlated atomic displacements, which efficiently scatter phonons. This mechanism is general and suggests a new avenue for the nanoscale engineering of materials to achieve low thermal conductivities for efficient thermoelectric converters and phase-change memory devices.
Source: europepmc · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Advanced Thermoelectric Materials and Devices · Thermal properties of materials · Phase-change materials and chalcogenides

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (43)

Show source-provided references
1. Minnich, A. J., Dresselhaus, M. S., Ren, Z. F. & Chen, G. Bulk nanostructured thermoelectric materials: current research and future prospects. Energy Environ. Sci. 2, 466–479 (2009).10.1039/b822664b ↗
2. Chen, G., Dresselhaus, M. S., Dresselhaus, G., Fleurial, J-P. & Caillat, T. Recent developments in thermoelectric materials. Int. Mater. Rev. 48, 45–66 (2003).10.1179/095066003225010182 ↗
3. Wood, C. Materials for thermoelectric energy conversion. Rep. Prog. Phys. 51, 459–539 (1988).10.1088/0034-4885/51/4/001 ↗
4. Goldsmid, H. J. Introduction to Thermoelectricity (Springer, 2010).10.1007/978-3-642-00716-3 ↗
5. Snyder, G. J. & Toberer, E. S. Complex thermoelectric materials. Nature Mater. 7, 105–114 (2008).10.1038/nmat2090 ↗
6. Siegrist, T., Merkelbach, P. & Wuttig, M. Phase change materials: challenges on the path to a universal storage device. Annu. Rev. Condens. Matter Phys. 3, 215–237 (2012).10.1146/annurev-conmatphys-020911-125105 ↗
7. Matsunaga, T. et al. Phase-change materials: vibrational softening upon crystallization and its impact on thermal properties. Adv. Funct. Mater. 21, 2232–2239 (2011).10.1002/adfm.201002274 ↗
8. Schneider, M. N., Rosenthal, T., Stiewe, C. & Oeckler, O. From phase-change materials to thermoelectrics? Z. Kristallogr. 225, 463–470 (2010).10.1524/zkri.2010.1320 ↗
9. Detemple, R., Wamwangi, D., Wuttig, M. & Bihlmayer, G. Identification of Te alloys with suitable phase change characteristics. Appl. Phys. Lett. 83, 2572–2574 (2003).10.1063/1.1608482 ↗
10. Hockings, E. F. The thermal conductivity of silver antimony telluride. J. Phys. Chem. Solids 10, 341–342 (1959).10.1016/0022-3697(59)90014-9 ↗
11. Wolfe, R., Wernick, J. H. & Haszko, S. E. Anomalous Hall effect in AgSbTe2 . J. Appl. Phys. 31, 1959–1964 (1960).10.1063/1.1735479 ↗
12. Morelli, D. T., Jovovic, V. & Heremans, J. P. Intrinsically minimal thermal conductivity in cubic I–V–VI2 semiconductors. Phys. Rev. Lett. 101, 035901 (2008).10.1103/PhysRevLett.101.035901 ↗
13. Nielsen, M. D., Ozolins, V. & Heremans, J-P. Lone pair electrons minimize lattice thermal conductivity. Energy Environ. Sci. 6, 570–578 (2013).10.1039/C2EE23391F ↗
14. Zhang, S., Zhu, T., Yang, S., Yu, C. & Zhao, X. Improved thermoelectric properties of AgSbTe2 based compounds with nanoscale Ag2Te in situ precipitates. Acta Mater. 58, 4160–4169 (2010).10.1016/j.actamat.2010.04.007 ↗
15. Jovovic, V. & Heremans, J. P. Measurements of the energy band gap and valence band structure of AgSbTe2 . Phys. Rev. B 77, 245204 (2008).10.1103/PhysRevB.77.245204 ↗
16. Hsu, K. F. et al. Cubic AgPbmSbTe2+m: bulk thermoelectric materials with high figure of merit. Science 303, 818–821 (2004).10.1126/science.1092963 ↗
17. Skrabek, E. A. & Trimmer, D. S. in CRC Handbook of Thermoelectrics (ed. Rowe, D. M.) 267–275 (CRC, 1995).
18. Ye, L-H. et al. First-principles study of the electronic, optical, and lattice vibrational properties of AgSbTe2 . Phys. Rev. B 77, 245203 (2008).10.1103/PhysRevB.77.245203 ↗
19. Lencer, D. et al. A map for phase-change materials. Nature Mater. 7, 972–977 (2008).10.1038/nmat2330 ↗
20. Shportko, K. et al. Resonant bonding in crystalline phase-change materials. Nature Mater. 7, 653–658 (2008).10.1038/nmat2226 ↗
21. Delaire, O. et al. Giant anharmonic phonon scattering in PbTe. Nature Mater. 10, 614–619 (2011).10.1038/nmat3035 ↗
22. Delaire, O. et al. Phonon softening and metallization of a narrow-gap semiconductor by thermal disorder. Proc. Natl Acad. Sci. USA 108, 4725–4730 (2011).10.1073/pnas.1014869108 ↗
23. Pang, J. W. L. et al. Phonon lifetime investigation of anharmonicity and thermal conductivity of UO2 by neutron scattering and theory. Phys. Rev. Lett. 110, 157401 (2013).10.1103/PhysRevLett.110.157401 ↗
24. Maier, R. G. Zur Kenntnis des Systems PbTe–AgSbTe2. Zeitschrift für Metallkunde 54, 311–312 (1963).
25. Marin, R-M., Brun, G. & Tedenac, J-C. Phase equilibria in the Sb2Te3–Ag2Te system J. Mater. Sci. 20, 730–735 (1985).10.1007/BF01026548 ↗
26. Sugar, J. & Medlin, D. Precipitation of Ag2Te in the thermoelectric material AgSbTe2 . J. All. Comp. 478, 75–82 (2009).10.1016/j.jallcom.2008.11.054 ↗
27. Geller, S. & Wernick, J. H. Ternary semiconducting compounds with sodium chloride-like structure—AgSbSe2, AgSbTe2, AgBiS2, AgBiSe2 . Acta Crystallogr. 12, 46–54 (1959).10.1107/S0365110X59000135 ↗
28. Quarez, E. et al. Nanostructuring, compositional fluctuations, and atomic ordering in the thermoelectric materials AgPbmSbTe2+m. The myth of solid solutions. J. Am. Chem. Soc. 127, 9177–9190 (2005).10.1021/ja051653o ↗
29. Sharma, P. A., Sugar, J. D. & Medlin, D. L. Influence of nanostructuring and heterogeneous nucleation on the thermoelectric figure of merit in AgSbTe2 . J. Appl. Phys. 107, 113716 (2010).10.1063/1.3446094 ↗
30. Sugar, J. & Medlin, D. Solid-state precipitation of stable and metastable layered compounds in thermoelectric AgSbTe2 . J. Mater. Sci. 46, 1668–1679 (2011).10.1007/s10853-010-4984-4 ↗
31. Hoang, K., Mahanti, S. D., Salvador, J. R. & Kanatzidis, M. G. Atomic ordering and gap formation in Ag–Sb-based ternary chalcogenides. Phys. Rev. Lett. 99, 156403 (2007).10.1103/PhysRevLett.99.156403 ↗
32. Barabash, S. V., Ozolins, V. & Wolverton, C. First-principles theory of competing order types, phase separation, and phonon spectra in thermoelectric AgPbmSbTem+2 alloys. Phys. Rev. Lett. 101, 155704 (2008).10.1103/PhysRevLett.101.155704 ↗
33. Barabash, S. V. & Ozolins, V. Order, miscibility, and electronic structure of Ag(Bi,Sb)Te2 alloys and (Ag,Bi,Sb)Te2 precipitates in rocksalt matrix: a first-principles study. Phys. Rev. B 81, 075212 (2010).10.1103/PhysRevB.81.075212 ↗
34. Manolikas, C. & Spyridelis, J. Electron microscopic study of polymorphism and defects in AgBiSe2 and AgBiS2 . Mater. Res. Soc. Bull. 12, 907–913 (1977).10.1016/0025-5408(77)90102-7 ↗
35. Abernathy, D. L. et al. Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source. Rev. Sci. Instrum. 83, 015114 (2012).10.1063/1.3680104 ↗
36. Ehlers, G., Podlesnyak, A. A., Niedziela, J. L., Iverson, E. B. & Sokol, P. E. The new cold neutron chopper spectrometer at the Spallation Neutron Source: design and performance. Rev. Sci. Instrum. 82, 085108 (2011).10.1063/1.3626935 ↗
37. Peierls, R. E. On the kinetic theory of thermal conduction in crystals. Ann. Phys. (Leipz.) Ser. 5, 1055–1101 (1929).10.1002/andp.19293950803 ↗
38. Slack, G. & Galginaitis, S. Thermal conductivity and phonon scattering by magnetic impurities in CdTe. Phys. Rev. 133, 253–268 (1964).10.1103/PhysRev.133.A253 ↗
39. Krumhansl, J. A. & Matthew, J. A. D. Scattering of long-wavelength phonons by point imperfections in crystals. Phys. Rev. 140, A1812–A1817 (1965).10.1103/PhysRev.140.A1812 ↗
40. Wolfe, J. P. Imaging Phonons: Acoustic Wave Propagation in Solids 1 (Cambridge Univ. Press, 1998).10.1017/CBO9780511665424 ↗
41. Biswas, K. et al. Strained endotaxial nanostructures with high thermoelectric figure of merit. Nature Chem. 3, 160–166 (2011).10.1038/nchem.955 ↗
42. Biswas, K. et al. High-performance bulk thermoelectrics with all-scale hierarchical architectures. Nature 489, 414–418 (2012).10.1038/nature11439 ↗
43. Pei, Y., Heinz, N. A., LaLonde, A. & Snyder, G. J. Combination of large nanostructures and complex band structure for high performance thermoelectric lead telluride. Energy Environ. Sci. 4, 3640–3645 (2011).10.1039/c1ee01928g ↗