Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites View Full Text


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2019-12

AUTHORS

Yinsheng Guo, Omer Yaffe, Trevor D. Hull, Jonathan S. Owen, David R. Reichman, Louis E. Brus

ABSTRACT

Lead-halide perovskites have emerged as promising materials for photovoltaic and optoelectronic applications. Their significantly anharmonic lattice motion, in contrast to conventional harmonic semiconductors, presents a conceptual challenge in understanding the genesis of their exceptional optoelectronic properties. Here we report a strongly temperature dependent luminescence Stokes shift in the electronic spectra of both hybrid and inorganic lead-bromide perovskite single crystals. This behavior stands in stark contrast to that exhibited by more conventional crystalline semiconductors. We correlate the electronic spectra with the anti-Stokes and Stokes Raman vibrational spectra. Dielectric solvation theories, originally developed for excited molecules dissolved in polar liquids, reproduce our experimental observations. Our approach, which invokes a classical Debye-like relaxation process, captures the dielectric response originating from the incipient anharmonicity of the LO phonon at about 20 meV (160 cm-1) in the lead-bromide framework. We reconcile this liquid-like model incorporating thermally-activated dielectric solvation with more standard solid-state theories of the emission Stokes shift in crystalline semiconductors. More... »

PAGES

1175

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/s41467-019-09057-5

DOI

http://dx.doi.org/10.1038/s41467-019-09057-5

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1112706415

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/30862815


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284 https://www.grid.ac/institutes/grid.21729.3f schema:alternateName Columbia University
285 schema:name Department of Chemistry, Columbia University, 10027, New York, NY, USA
286 rdf:type schema:Organization
 




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