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Isotopic effects on phonon anharmonicity in layered van der Waals crystals: Isotopically pure hexagonal boron nitride

AuthorsCuscó, Ramón CSIC ORCID ; Artús, Lluís CSIC ORCID ; Edgar, J. H.; Liu, Song; Cassabois, Guillaume; Gil, Bernard
Issue DateApr-2018
PublisherAmerican Physical Society
CitationPhysical Review B, 97(15): Article number 155435 (2018)
AbstractHexagonal boron nitride (h-BN) is a layered crystal that is attracting a great deal of attention as a promising material for nanophotonic applications. The strong optical anisotropy of this crystal is key to exploit polaritonic modes for manipulating light-matter interactions in 2D materials. h-BN has also great potential for solid-state neutron detection and neutron imaging devices, given the exceptionally high thermal neutron capture cross section of the boron-10 isotope. A good knowledge of phonons in layered crystals is essential for harnessing long-lived phonon-polariton modes for nanophotonic applications and may prove valuable for developing solid-state BN10 neutron detectors with improved device architectures and higher detection efficiencies. Although phonons in graphene and isoelectronic materials with a similar hexagonal layer structure have been studied, the effect of isotopic substitution on the phonons of such lamellar compounds has not been addressed yet. Here we present a Raman scattering study of the in-plane high-energy Raman active mode on isotopically enriched single-crystal h-BN. Phonon frequency and lifetime are measured in the 80-600-K temperature range for B10-enriched, B11-enriched, and natural composition high quality crystals. Their temperature dependence is explained in the light of perturbation theory calculations of the phonon self-energy. The effects of crystal anisotropy, isotopic disorder, and anharmonic phonon-decay channels are investigated in detail. The isotopic-induced changes in the phonon density of states are shown to enhance three-phonon anharmonic decay channels in B10-enriched crystals, opening the possibility of isotope tuning of the anharmonic phonon decay processes. © 2018 American Physical Society.
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