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Abstract Amorphous chalcogenide alloys are key materials for data storage and energy scavenging applications due to their large non-linearities in optical and electrical properties as well as low vibrational thermal conductivities. Here, we report on a mechanism to suppress the thermal transport in a representative amorphous chalcogenide system, silicon telluride (SiTe), by nearly an order of magnitude via systematically tailoring the cross-linking network among the atoms. As such, we experimentally demonstrate that in fully dense amorphous SiTe the thermal conductivity can be reduced to as low as 0.10 ± 0.01 W m −1 K −1 for high tellurium content with a density nearly twice that of amorphous silicon. Using ab-initio simulations integrated with lattice dynamics, we attribute the ultralow thermal conductivity of SiTe to the suppressed contribution of extended modes of vibration, namely propagons and diffusons. This leads to a large shift in the mobility edge - a factor of five - towards lower frequency and localization of nearly 42% of the modes. This localization is the result of reductions in coordination number and a transition from over-constrained to under-constrained atomic network.more » « less
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Li, Wu ; Lindsay, L. ; Broido, D. A. ; Stewart, Derek A. ; Mingo, Natalio ( , Physical Review B)
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Chen, Xi ; Weathers, Annie ; Carrete, Jesús ; Mukhopadhyay, Saikat ; Delaire, Olivier ; Stewart, Derek A. ; Mingo, Natalio ; Girard, Steven N. ; Ma, Jie ; Abernathy, Douglas L. ; et al ( , Nature Communications)