Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.092
Publication date: 22nd December 2022
Silver phenylselenolate (AgSePh) and silver phenyltellurolate (AgTePh) are novel two-dimensional (2D) van der Waals semiconductors. In contrast to 2D layered perovskites and transition metal dichalcogenides, AgSePh and AgTePh have strong covalent interaction between organic and inorganic components, becoming truly hybrid organic-inorganic semiconductors. However, despite having the similar crystal structure, composition and absorption characteristics, AgSePh and AgTePh exhibit strikingly different light emission characteristics. Whereas AgSePh exhibit narrow, fast luminescence with a minimal Stokes shift that tracks the temperature-dependent shifting of the lowest-energy excitonic absorption resonance, AgTePh exhibits comparatively slow, significantly broadened luminescence with large Stokes shift that does not track the shifting of excitonic absorption resonance peak with changing temperature. In this presentation, we will present the synthesis, structure and excitonic optical properties of AgSePh and AgTePh films. Furthermore, we will discuss different physical mechanisms underlying light emission in AgSePh and AgTePh. Using time-resolved and temperature-dependent optical spectroscopy, combined with sub-gap photoexcitation spectroscopy, we will show that exciton dynamics in AgTePh are dominated by intrinsic self-trapping behavior, whereas dynamics in AgTePh are dominated by interaction of band edge excitons with extrinsic defect states. Finally, we will show tunable excitonic properties in AgSe1-xTexPh alloys depending on composition.
Materials synthesis and characterization was supported by the U.S. Army Research Office under Award Number W911NF20-1-0200. The electronic structure calculations were supported in part by the United States Department of Energy under grant number DE-NA0003965. Spectroscopic studies were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award Number DESC0019345. W.S.L. was partially supported by the Seoul Broadcasting System Foundation Overseas Doctoral Program Scholarship. E.R.P. was supported by the U.S. Department of Defense through the National Defense Science & Engineering Graduate (NDSEG) Fellowship Program. T.S. was supported by AGC Inc. (formerly Asahi Glass Co., Ltd.)
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