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Coherent Exciton-Lattice Dynamics in a 2D Metal Organochalcogenolate Semiconductor
- Publication Year :
- 2023
-
Abstract
- Hybrid organic-inorganic nanomaterials can exhibit transitional behavior that deviates from models developed for all-organic or all-inorganic materials systems. Here, we reveal the complexity of exciton-phonon interactions in a recently discovered 2D layered hybrid organic-inorganic semiconductor, silver phenylselenolate (AgSePh). Using femtosecond resonant impulsive vibrational spectroscopy and non-resonant Raman scattering, we measure multiple hybrid organic-inorganic vibrational modes and identify a subset of these modes that strongly couple to the electronic excited state. 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 fine-structure splitting and temperature-dependent peak-shifting/linewidth-broadening suggests 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.
- Subjects :
- Condensed Matter - Materials Science
Physics - Chemical Physics
Subjects
Details
- Database :
- arXiv
- Publication Type :
- Report
- Accession number :
- edsarx.2310.08393
- Document Type :
- Working Paper