First-principles prediction of infrared phonon and dielectric function in biaxial hyperbolic van der Waals crystal α-MoO3

Zhen Tong, Traian Dumitrică, Thomas Frauenheim

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Layered biaxial hyperbolic molybdenum trioxide (α-MoO3) with weak van der Waals (vdW) interlayer bonding recently received extensive attention due to its anisotropic dielectric response to infrared (IR) radiation, which couples to the lattice vibrations and allows for manipulating the radiative energy transport. However, the understanding of IR-active phonon modes and dielectric function of it has not yet been fully achieved. Here, by utilizing mode-level first-principles analysis based on density functional theory (DFT), the phonon modes contributing to the IR dielectric response of α-MoO3are fully determined. The anisotropic IR-active modes are identified from lattice vibration analysis, allowing for a clear evaluation of the IR absorption contribution from the weak or strong IR phonon modes. By further employing anharmonic-lattice dynamics calculations, the damping of the corresponding IR modes is directly obtained. This approach enables predictions of IR optical properties without any fitting or assumed parameters. Our predictions bridge the scientific gap of comprehensively understanding the unreported IR-active phonon modes of α-MoO3and overall agree well with available experimental data, placing our DFT-based method at a privileged stage for accurately predicting the IR optical properties of α-MoO3. These comprehensive understandings of the IR phonons and dielectric properties of α-MoO3pave the way for nanophotonic devices with tunable functionalities and enable design of α-MoO3for advanced optical devices.

Original languageEnglish (US)
Pages (from-to)19627-19635
Number of pages9
JournalPhysical Chemistry Chemical Physics
Issue number35
StatePublished - Sep 15 2021

Bibliographical note

Funding Information:
We would like to thank Dr C. Y. Yam for valuable discussions. Simulations were performed at the Tainhe2-JK of Beijing Computational Science Research Center (CSRC). Z. T. acknowledges the support by China Postdoctoral Science Foundation (Grant No. 2020M680127), Guangdong Basic and Applied Basic Research Foundation (Grants No. 2020A1515110838 and 2021A1515011688), and Shenzhen Science and Technology Program (Grant No. RCBS20200714114919142). T. F. acknowledges the support from DFG FR-2833/7 and National Natural Science Foundation of China (Grant No. U1930402).

Publisher Copyright:
© the Owner Societies 2021.

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