Tailoring phonon-driven responses in α-MoO3 through isotopic enrichment
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2026
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| author | Arnaud, Thiago S. Spangler, Ryan W. Georgaras, Johnathan D. Haber, Jonah B. Hirt, Daniel Obst, Maximilian Álvarez-Pérez, Gonzalo Long III, Mackey Kaps, Felix G. Wetzel, Jakob Ragle, Courtney Buchner, John E. Kim, Youngji Senarath, Aditha S. Niemann, Richarda He, Mingze Carini, Giulia Arregui-Leon, Unai Behera, Akash C. Bangari, Ramachandra Sahoo, Nihar Brumby, Niels C. Klopf, J. Michael Wolf, Martin Eng, Lukas M. Kehr, Susanne C. Folland, Thomas G. Paarmann, Alexander Hopkins, Patrick E. Jornada, Felipe Maria, Jon-Paul Caldwell, Joshua D. |
| author_facet | Arnaud, Thiago S. Spangler, Ryan W. Georgaras, Johnathan D. Haber, Jonah B. Hirt, Daniel Obst, Maximilian Álvarez-Pérez, Gonzalo Long III, Mackey Kaps, Felix G. Wetzel, Jakob Ragle, Courtney Buchner, John E. Kim, Youngji Senarath, Aditha S. Niemann, Richarda He, Mingze Carini, Giulia Arregui-Leon, Unai Behera, Akash C. Bangari, Ramachandra Sahoo, Nihar Brumby, Niels C. Klopf, J. Michael Wolf, Martin Eng, Lukas M. Kehr, Susanne C. Folland, Thomas G. Paarmann, Alexander Hopkins, Patrick E. Jornada, Felipe Maria, Jon-Paul Caldwell, Joshua D. |
| contents | The implementation of polaritonic materials into nanoscale devices requires selective tuning of parameters to realize desired spectral or thermal responses. One robust material is α-MoO3, which as an orthorhombic crystal boasts three distinct phonon dispersions, providing 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) are 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 their Q- factors are reported. A Q-factor maxima increase of ~50 % along the [100] in the RB2 and ~100 % along the [001] in the RB3 are reported for HPhPs supported in 98Mo18O3. Observations in both real and Fourier space of higher-order HPhP modes propagating in single slabs of isotopically enriched α-MoO3 without the use of a subdiffractional surface scatterer are presented here. This work illustrates the tunability of α-MoO3 for thermal and nanophotonic applications. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2601_02570 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Tailoring phonon-driven responses in α-MoO3 through isotopic enrichment Arnaud, Thiago S. Spangler, Ryan W. Georgaras, Johnathan D. Haber, Jonah B. Hirt, Daniel Obst, Maximilian Álvarez-Pérez, Gonzalo Long III, Mackey Kaps, Felix G. Wetzel, Jakob Ragle, Courtney Buchner, John E. Kim, Youngji Senarath, Aditha S. Niemann, Richarda He, Mingze Carini, Giulia Arregui-Leon, Unai Behera, Akash C. Bangari, Ramachandra Sahoo, Nihar Brumby, Niels C. Klopf, J. Michael Wolf, Martin Eng, Lukas M. Kehr, Susanne C. Folland, Thomas G. Paarmann, Alexander Hopkins, Patrick E. Jornada, Felipe Maria, Jon-Paul Caldwell, Joshua D. Materials Science Mesoscale and Nanoscale Physics The implementation of polaritonic materials into nanoscale devices requires selective tuning of parameters to realize desired spectral or thermal responses. One robust material is α-MoO3, which as an orthorhombic crystal boasts three distinct phonon dispersions, providing 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) are 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 their Q- factors are reported. A Q-factor maxima increase of ~50 % along the [100] in the RB2 and ~100 % along the [001] in the RB3 are reported for HPhPs supported in 98Mo18O3. Observations in both real and Fourier space of higher-order HPhP modes propagating in single slabs of isotopically enriched α-MoO3 without the use of a subdiffractional surface scatterer are presented here. This work illustrates the tunability of α-MoO3 for thermal and nanophotonic applications. |
| title | Tailoring phonon-driven responses in α-MoO3 through isotopic enrichment |
| topic | Materials Science Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2601.02570 |