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Elementary excitations, such as in-plane anisotropic phonons and phonon polaritons (PhPs), in α-MoO3 play key roles in its outstanding physical properties like high carrier mobility and ultralow phonon thermal conductivity ( κP). Understanding the excitation mechanisms like phonon–phonon interactions is the most fundamental step to further applications. Here, we report on the systematic Raman investigations on phonon anisotropy and anharmonicity of representative Mo–O stretching vibration phonon modes (SVPMs) in physical vapor deposition (PVD)-grown α-MoO3 flakes. Polarizations of SVPMs verify the phonon anisotropy. The abnormal temperature dependence of SVPMs reveals that giant quartic-phonon decay dominates the phonon anharmonicity in α-MoO3. An ultrashort phonon lifetime of ~ 0.34 ps gives evidence of theoretically predicted ultralow κP in α-MoO3. Our findings give deep insight into the phonon–phonon interactions in α-MoO3 and provide an indicator for its extreme thermal device applications.


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Giant quartic-phonon decay in PVD-grown α-MoO3 flakes

Show Author's information Yongsong Wang1,2Xiao Guo1,2Siwen You1,2Junjie Jiang2Zihan Wang2Fangping Ouyang2Han Huang1,2( )
School of Physics and Electronics, Hunan Key Laboratory of Nanophotonics and Devices, Central South University, Changsha 410083, China
School of Physics and Electronics, Hunan Key Laboratory of Super-microstructure and Ultrafast Process, Central South University, Changsha 410083, China

Abstract

Elementary excitations, such as in-plane anisotropic phonons and phonon polaritons (PhPs), in α-MoO3 play key roles in its outstanding physical properties like high carrier mobility and ultralow phonon thermal conductivity ( κP). Understanding the excitation mechanisms like phonon–phonon interactions is the most fundamental step to further applications. Here, we report on the systematic Raman investigations on phonon anisotropy and anharmonicity of representative Mo–O stretching vibration phonon modes (SVPMs) in physical vapor deposition (PVD)-grown α-MoO3 flakes. Polarizations of SVPMs verify the phonon anisotropy. The abnormal temperature dependence of SVPMs reveals that giant quartic-phonon decay dominates the phonon anharmonicity in α-MoO3. An ultrashort phonon lifetime of ~ 0.34 ps gives evidence of theoretically predicted ultralow κP in α-MoO3. Our findings give deep insight into the phonon–phonon interactions in α-MoO3 and provide an indicator for its extreme thermal device applications.

Keywords: layered materials, anisotropy, synthesis, phonon–phonon coupling, ultralow phonon thermal conductivity

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Publication history
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Acknowledgements

Publication history

Received: 28 April 2022
Revised: 06 June 2022
Accepted: 01 July 2022
Published: 05 August 2022
Issue date: January 2023

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

We acknowledge the financial support from the National Natural Science Foundation of China (NSFC, No. 11874427).

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