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More than 500 abstracts submitted from over 50 countries


Featuring many Nobel Laureates and other Distinguished Guests

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Oral Presentations


SESSION:
SolidStateChemistryTuePM4-R7
Kanatzidis International Symposium (4th Intl. Symp. on Materials/Solid State Chemistry and Nanoscience for Sustainable Development)
Tue. 22 Oct. 2024 / Room: Ariadni A
Session Chairs: Omar Farha; Student Monitors: TBA

17:30: [SolidStateChemistryTuePM413] OS Invited
GIANT BIREFRINGENCE ACHIEVED VIA HYDROGEN BOND-CLICK REACTION FOR ENHANCED COPLANARITY LONG-RANGE ANION CORRELATIONS MEDIATING DYNAMIC ANHARMONICITY AND CONTRIBUTING TO GLASSY THERMAL CONDUCTIVITY IN WELL-ORDERED K2Ag4Se3
Li-Ming Wu1
1Beijing Normal University, Beijing, China
Paper ID: 448 [Abstract]

The realization of ultralow thermal conductivity in a well-ordered structure is crucial for crystalline materials which consider heat conduction properties to be primary in design. We report herein an extremely low (0.32‒0.25 Wm-1K-1) and glassy temperature dependence (300‒600 K) of lattice thermal conductivity in a monoclinic K2Ag4Se3. By applying a unified theory of thermal transport, we reveal that K2Ag4Se3 features a complex phonon scattering mechanism. Delocalized vibrational correlations lead to synergistic inhibition of both propagating and wave-like heat conduction through polarization transmission. Density functional theory calculations reveal that long-range correlated Se vibrations, enhanced by delocalized hole carriers, promote interlayer lattice shearing. This shearing induces dynamically competitive expressions of different orders of anharmonicity, ultimately leading to full-spectrum phonon bunching as the temperature increases. These correlated interactions cause Se anions to vibrate together as a cluster in the low frequency region, resulting in short phonon lifetimes, low group velocities, and a large scattering phase space, which ultimately suppresses both intra- and inter-band phonon transfers. Moreover, these findings have been experimentally confirmed through low-temperature heat capacity measurements and in situ Raman spectroscopy. The insights gained from this work will advance the design of crystalline materials with tailored thermal properties.

References:
[1] Li, F.; Liu, X.; Li, S. R.; Zhang, X. F.; Ma, N.; Li, X. J.; Lin, X. Y.; Chen, L.; Wu, H. J.; Wu, L.-M. Rare Three-Valence-Band Convergence Leading to Ultrahigh Thermoelectric Performance in All-Scale Hierarchical Cubic SnTe. Energy Environ. Sci. 2024, 17, 158–172.
[2] Jia, F.; Zhao, S.; Wu, J.; Chen, L.; Liu, T.-H.; Wu, L.-M. Cu3BiS3: Two-Dimensional Coordination Induces Out-of-Plane Phonon Scattering Enabling Ultralow Thermal Conductivity. Angew. Chem. Int. Ed. 2023, 62, e202315642.
[3] Li, F.; Liu, X.; Ma, N.; Yang, Y. C.; Yin, J. P.; Chen, L.; Wu, L.-M. Overdamped Phonon Diffusion and Nontrivial Electronic Structure Leading to a High Thermoelectric Figure of Merit in KCu5Se3. J. Am. Chem. Soc. 2023, 145, 14981−14993.


18:50 GALA DINNER/AWARDS CEREMONY/SHOW - Marika A Ballroom