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Tailoring Phonon-Driven Responses in α-MoO 3 through Isotopic Enrichment
Journal article   Open access   Peer reviewed

Tailoring Phonon-Driven Responses in α-MoO 3 through Isotopic Enrichment

Thiago S Arnaud, Ryan W Spangler, Johnathan D Georgaras, Jonah B Haber, Daniel Hirt, Maximilian Obst, Gonzalo Álvarez-Pérez, Mackey Long Iii, Felix G Kaps, Jakob Wetzel, …
Advanced materials (Weinheim), Vol.38(39), e73629
06/11/2026
DOI: 10.1002/adma.73629
PMID: 42273746
url
https://doi.org/10.1002/adma.73629View
Published (Version of record) Open Access

Abstract

The implementation of polaritonic materials into nanoscale devices requires selective tuning of parameters to realize desired spectral or thermal responses. One robust material, α-MoO3, an orthorhombic crystal boasting three distinct phonon dispersions, provides three polaritonic dispersions of hyperbolic phonon polaritons (HPhPs) across the mid-infrared (MIR). Here, the tunability of both optical and thermal responses in isotopically enriched α-MoO3 (98MoO3, Mo18O3, and 98Mo18O3) is explored. A uniform ∼5% spectral redshift from 18O enrichment is observed in both Raman- and IR-active TO phonons. Both the in- and out-of-plane thermal conductivities for the isotopic variations are reported. Ab initio calculations both replicate experimental findings and analyze the select-mode three-phonon scattering contributions. The HPhPs from each isotopic variation are probed with s-SNOM, and we report an HPhP Q-factor maxima increase in 98Mo18O3 of ∼50% along the [100] in the RB2 and ∼100% along the [001] in the RB3 with respect to 98MoO3. Observations in both real and Fourier space of higher-order HPhP modes propagating in slabs of isotopically enriched α-MoO3 without the use of a subdiffractional surface scatterer are presented here. This work establishes the dual-element isotope enrichment of α-MoO3 as an intrinsic strategy to design optical, thermal, and polaritonic properties.
density functional perturbation theory acoustic phonon isotopic substitution mid‐infrared thermal conductivity hyperbolic phonon polaritons optical phonon

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