Eric R. Powers , Watcharaphol Paritmongkol , Dillon C. Yost , Woo Seok Lee , Jeffrey C. Grossman , William A. Tisdale
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Coherent exciton-lattice dynamics in a 2D metal organochalcogenolate semiconductor
We reveal coherent exciton-phonon interactions in the two-dimensional (2D) layered hybrid organic-inorganic semiconductor silver phenylselenolate (AgSePh). Using femtosecond resonant impulsive vibrational spectroscopy and non-resonant Raman scattering, we identify multiple hybrid organic-inorganic vibrational modes that strongly couple to the excitonic transitions and characterize their behavior. Calculations by density functional perturbation theory show that these strongly coupled modes exhibit large out-of-plane silver atomic motions and silver-selenium spacing displacements. Moreover, analysis of photoluminescence spectral splitting and temperature-dependent peak shifting/linewidth broadening reveals that light emission in AgSePh is most strongly affected by a compound 100 cm−1 mode involving the wagging motion of phenylselenolate ligands and accompanying metal-chalcogen stretching. Finally, red shifting of vibrational modes with increasing temperature reveals a high degree of anharmonicity arising from non-covalent interactions between phenyl rings. These findings reveal the unique effects of hybrid vibrational modes in organic-inorganic semiconductors and motivate future work aimed at specifically engineering such interactions through chemical and structural modification.
期刊介绍:
Matter, a monthly journal affiliated with Cell, spans the broad field of materials science from nano to macro levels,covering fundamentals to applications. Embracing groundbreaking technologies,it includes full-length research articles,reviews, perspectives,previews, opinions, personnel stories, and general editorial content.
Matter aims to be the primary resource for researchers in academia and industry, inspiring the next generation of materials scientists.