Your browser doesn't support javascript.
loading
Exciton polaron formation and hot-carrier relaxation in rigid Dion-Jacobson-type two-dimensional perovskites.
Biswas, Somnath; Zhao, Ruyan; Alowa, Fatimah; Zacharias, Marios; Sharifzadeh, Sahar; Coker, David F; Seferos, Dwight S; Scholes, Gregory D.
Afiliación
  • Biswas S; Department of Chemistry, Princeton Uiversity, Princeton, NJ, USA.
  • Zhao R; Department of Chemistry, University of Toronto, Toronto, Ontario, Canada.
  • Alowa F; Division of Materials Science and Engineering, Boston University, Boston, MA, USA.
  • Zacharias M; Université de Rennes, INSA Rennes, CNRS, Institut FOTON - UMR 6082, F-35000, Rennes, France.
  • Sharifzadeh S; Department of Electrical and Computer Engineering, Boston University, Boston, MA, USA.
  • Coker DF; Department of Chemistry, Boston University, Boston, MA, USA.
  • Seferos DS; Department of Chemistry, University of Toronto, Toronto, Ontario, Canada. dwight.seferos@utoronto.ca.
  • Scholes GD; Department of Chemistry, Princeton Uiversity, Princeton, NJ, USA. gscholes@princeton.edu.
Nat Mater ; 23(7): 937-943, 2024 Jul.
Article en En | MEDLINE | ID: mdl-38755291
ABSTRACT
The efficiency of two-dimensional Dion-Jacobson-type materials relies on the complex interplay between electronic and lattice dynamics; however, questions remain about the functional role of exciton-phonon interactions. Here we establish the robust polaronic nature of the excitons in these materials at room temperature by combining ultrafast spectroscopy and electronic structure calculations. We show that polaronic distortion is associated with low-frequency (30-60 cm-1) lead iodide octahedral lattice motions. More importantly, we discover how targeted ligand modification of this two-dimensional perovskite structure manipulates exciton-phonon coupling, exciton polaron population and carrier cooling. At high excitation density, stronger exciton-phonon coupling increases the hot-carrier lifetime, forming a hot-phonon bottleneck. Our study provides detailed insight into the exciton-phonon coupling and its role in carrier cooling in two-dimensional perovskites relevant for developing emerging hybrid semiconductor materials with tailored properties.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Mater Asunto de la revista: CIENCIA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Mater Asunto de la revista: CIENCIA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido