Determining van der Waals materials' optical and polaritonic properties using cryogenic FTIR micro-spectroscopy

Abstract

Van-der-Waals materials have been shown to support numerous exotic polaritonic phenomena originating from their layered structures and associated vibrational and electronic properties. This includes emergent polaritonic phenomena, including hyperbolicity and exciton-polariton formation. However, many van-der-Waals materials' unique properties are most prominent at cryogenic temperatures. This presents a particular challenge for polaritonics research, as reliable optical constant data is required for understanding light-matter coupling. For infrared polaritonics (3-100um), the small size of exfoliated flakes makes conventional ellipsometry impossible. This paper presents a cryogenic Fourier transform infrared microscope design constructed entirely from off-the-shelf components and fitting procedures for determining optical constants. We use this microscope to present the first temperature-dependent characterization of the optical properties of hexagonal boron nitride grown with isotopically pure boron. We show that Fabry Perot-type resonances close to the transverse optical phonon show the key temperature-dependent tuning of several parameters. Our full analysis of the infrared dielectric function shows small but significant tuning of the optical constants, which is highly consistent with Raman data from the literature. We then use this dielectric data to perform and analyze the polariton propagation properties, which agree extremely well with published cryogenic scattering-type nearfield microscopy results. In addition to the insights gained into hyperbolic polaritons in hBN, our paper represents a transferable framework for characterizing exfoliated infrared polaritonic materials and other infrared devices. This could accelerate discoveries in other material systems, especially those that are spatially inhomogeneous or cannot be prepared as large single crystals.