期刊
NATURE MATERIALS
卷 18, 期 4, 页码 349-+出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41563-018-0262-7
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资金
- EU Horizon 2020 via a Marie Sklodowska Curie Fellowship (Global) [705874]
- Natural Sciences and Engineering Research Council of Canada
- Fond Quebecois pour la Recherche: Nature et Technologies
- National Science Foundation [1838276]
- School of Chemistry and Biochemistry of Georgia Institute of Technology
- College of Science of Georgia Institute of Technology
- Interuniversity Attraction Pole programme of the Belgian Federal Science Policy Office [PAI 6/27]
- FNRS-F.R.S
- Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) [2.5020.11]
- Marie Curie Actions (MSCA) [705874] Funding Source: Marie Curie Actions (MSCA)
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1838276] Funding Source: National Science Foundation
Hybrid organic-inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency (less than or similar to 50 cm(-1)) optical phonons involving motion in the lead iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight into the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.
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