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Hyperbolic phonon polaritons in optically uniaxial hexagonal boron nitride (hBN) have shown considerable potential for manipulating light on the deep‐subwavelength scale, but the inherent in‐plane isotropy of hBN hinders their further application in planar polariton meta‐optics. Engineering these polaritons to achieve ultraconfined in‐plane anisotropic propagation is of scientific significance for facilitating light–matter interactions toward an extreme scale. Here, the polariton features are systematically investigated in a vertically stacked van der Waals heterostructure consisting of hBN and tellurium (Te), a highly birefringent van der Waals crystal in the mid‐infrared region. Polaritons in this heterostructure exhibit Te‐thickness‐dependent anisotropic dispersion, and the configurable in‐plane anisotropy and enhanced field confinement are experimentally demonstrated using scanning near‐field optical microscopy. It is concluded that these findings contribute to the fundamental understanding of anisotropic polaritons in hBN van der Waals heterostructures, providing a practical avenue for effectively engineering anisotropic PhPs in an intrinsically isotropic van der Waals material. [ABSTRACT FROM AUTHOR]

The effect of birefringence in anisotropic materials has been a long‐term issue for polarized Raman scattering. In this work, the polarization‐dependent Raman scattering in anisotropically birefringent materials is modeled with birefringence considered in the fundamental polarization selection rule. The birefringence‐induced polarization transformation is treated as a tensor in the calculation of Raman scattering intensity. The validity of this theory is further demonstrated in experiments by taking angle‐resolved polarized Raman measurements on the basal and cross planes of α‐MoO3—a typical biaxial van der Waals crystal with strong in‐plane and out‐of‐plane anisotropy. The anomalous angular dependency of polarized Raman scattering intensity can be well reproduced by the modified theoretical model with fitted real‐valued Raman tensors and birefringence‐related parameters. It can be concluded that this work can provide a valuable reference and guidance for quantitative analyses of anisotropic materials by using polarization‐resolved Raman scattering spectroscopy. [ABSTRACT FROM AUTHOR]

The effect of birefringence in anisotropic materials has been a long‐term issue for polarized Raman scattering. In this work, the polarization‐dependent Raman scattering in anisotropically birefringent materials is modeled with birefringence considered in the fundamental polarization selection rule. The birefringence‐induced polarization transformation is treated as a tensor in the calculation of Raman scattering intensity. The validity of this theory is further demonstrated in experiments by taking angle‐resolved polarized Raman measurements on the basal and cross planes of α‐MoO3—a typical biaxial van der Waals crystal with strong in‐plane and out‐of‐plane anisotropy. The anomalous angular dependency of polarized Raman scattering intensity can be well reproduced by the modified theoretical model with fitted real‐valued Raman tensors and birefringence‐related parameters. It can be concluded that this work can provide a valuable reference and guidance for quantitative analyses of anisotropic materials by using polarization‐resolved Raman scattering spectroscopy. [ABSTRACT FROM AUTHOR]

The recent discovery of in‐plane hyperbolic phonon polaritons in biaxial polar crystal—α‐MoO3, has aroused a huge research upsurge on anisotropic photonic quasiparticles in van der Waals materials. The physical origin of these highly anisotropic phonon polaritons is attributed to the strong anisotropy of crystal phonons. However, the orientation‐dependent phonon modes have not been fully understood from crystallographic point of view. This work systematically performs in situ angle‐resolved polarized Raman spectroscopy on α‐MoO3 to investigate its anisotropic photo‐phonon interactions. The sample orientation and Raman tensors are unambiguously determined under different polarization configurations. Specifically, the in‐plane anisotropic phonon modes of α‐MoO3 can be well characterized from the highly polarization‐dependent Raman‐active modes with periodic intensity variation. It can be concluded that these findings cannot only offer a better understanding of anisotropic phonon modes in α‐MoO3, but also provide a valuable reference for other anisotropic van der Waals crystals. [ABSTRACT FROM AUTHOR]

The recent discovery of in‐plane hyperbolic phonon polaritons in biaxial polar crystal—α‐MoO3, has aroused a huge research upsurge on anisotropic photonic quasiparticles in van der Waals materials. The physical origin of these highly anisotropic phonon polaritons is attributed to the strong anisotropy of crystal phonons. However, the orientation‐dependent phonon modes have not been fully understood from crystallographic point of view. This work systematically performs in situ angle‐resolved polarized Raman spectroscopy on α‐MoO3 to investigate its anisotropic photo‐phonon interactions. The sample orientation and Raman tensors are unambiguously determined under different polarization configurations. Specifically, the in‐plane anisotropic phonon modes of α‐MoO3 can be well characterized from the highly polarization‐dependent Raman‐active modes with periodic intensity variation. It can be concluded that these findings cannot only offer a better understanding of anisotropic phonon modes in α‐MoO3, but also provide a valuable reference for other anisotropic van der Waals crystals. [ABSTRACT FROM AUTHOR]