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Highly Mobile Large Polarons in Black Phase CsPbI<sub>3</sub>

Heng Zhang, Elke Debroye, Julian A. Steele, Maarten B. J. Roeffaers, Johan Hofkens, Hai I. Wang, Mischa Bonn

2021ACS Energy Letters64 citationsDOIOpen Access PDF

Abstract

We report the band-like\ntransport of photogenerated charge carriers\nwithin all-inorganic black γ-phase CsPbI&lt;sub&gt;3&lt;/sub&gt; (γ-CsPbI&lt;sub&gt;3&lt;/sub&gt;) thin films, with local mobilities up to 270 ± 44 cm&lt;sup&gt;2&lt;/sup&gt;V&lt;sup&gt;–1&lt;/sup&gt;s&lt;sup&gt;–1&lt;/sup&gt; recorded using\nterahertz (THz) spectroscopy at room temperature. Temperature-dependent,\nhigh-frequency photoconductivity measurements indicate that large\npolaron formation governs charge carrier transport, following the\nFeynman polaron model. The mobility values derived using THz spectroscopy\nare nearly 1 order of magnitude higher than that reported for hybrid\norganic–inorganic lead halide perovskites and approach the\ntheoretical limit for polarons scattering from longitudinal optical\n(LO) phonons. Our results identify γ-CsPbI&lt;sub&gt;3&lt;/sub&gt; as a\nfascinating all-inorganic perovskite semiconductor with high charge\ncarrier mobility for optoelectronics and reveal the effect of polaron\nformation on charge transport properties.

Topics & Concepts

PolaronCharge carrierPerovskite (structure)PhotoconductivityElectron mobilityPhononSemiconductorCondensed matter physicsTerahertz radiationSpectroscopyMaterials scienceTerahertz spectroscopy and technologyScatteringPhase (matter)ChemistryOptoelectronicsChemical physicsPhysicsElectronOpticsCrystallographyQuantum mechanicsOrganic chemistryPerovskite Materials and ApplicationsChalcogenide Semiconductor Thin Films2D Materials and Applications