Ruddlesden-Popper chalcogenides push the limit of mechanical stiffness and glass-like thermal conductivity in single crystals

Md Shafkat Bin Hoque, Eric R. Hoglund, Boyang Zhao, Bao De-Liang, Hao Zhou, Sandip Thakur, Eric Osei-Agyemang, Khalid Hattar, Ethan A. Scott, Mythili Surendran, John A. Tomko, John T. Gaskins, Kiumars Aryana, Sara Makarem, Adie Alwen, Andrea M. Hodge, Ganesh Balasubramanian, Ashutosh Giri, Tianli Feng, Jordan A. Hachtel, Jayakanth Ravichandran (), Sokrates T. Pantelides () and Patrick E. Hopkins ()
Additional contact information
Md Shafkat Bin Hoque: University of Virginia
Eric R. Hoglund: University of Virginia
Boyang Zhao: University of Southern California
Bao De-Liang: Vanderbilt University
Hao Zhou: University of Utah
Sandip Thakur: University of Rhode Island
Eric Osei-Agyemang: The State University of New York
Khalid Hattar: University of Tennessee
Ethan A. Scott: University of Virginia
Mythili Surendran: University of Southern California
John A. Tomko: University of Virginia
John T. Gaskins: Laser thermal analysis
Kiumars Aryana: University of Virginia
Sara Makarem: University of Virginia
Adie Alwen: University of Southern California
Andrea M. Hodge: University of Southern California
Ganesh Balasubramanian: University of New Haven
Ashutosh Giri: University of Rhode Island
Tianli Feng: University of Utah
Jordan A. Hachtel: Oak Ridge National Laboratory
Jayakanth Ravichandran: University of Southern California
Sokrates T. Pantelides: Vanderbilt University
Patrick E. Hopkins: University of Virginia

Nature Communications, 2025, vol. 16, issue 1, 1-8

Abstract: Abstract Insulating materials featuring ultralow thermal conductivity for diverse applications also require robust mechanical properties. Conventional thinking, however, which correlates strong bonding with high atomic-vibration-mediated heat conduction, led to diverse weakly bonded materials that feature ultralow thermal conductivity and low elastic moduli. One must, therefore, search for strongly-bonded single crystals in which heat transport is impeded by other means. Here, we report intrinsic, glass-like, ultralow thermal conductivity and ultrahigh elastic-modulus/thermal-conductivity ratio in single-crystalline Ruddlesden-Popper Ban+1ZrnS3n+1, n = 2, 3, which are derivatives of BaZrS3. Their key features are strong anharmonicity and intra-unit-cell rock-salt blocks. The latter produce strongly bonded intrinsic superlattices, impeding heat conduction by broadband reduction of phonon velocities and mean free paths and concomitant strong phonon localization. The present study initiates a paradigm of “mechanically stiff phonon glasses”.

Date: 2025
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DOI: 10.1038/s41467-025-61078-5

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