Tuning Hot Carrier Cooling Dynamics by Dielectric Confinement in Two-Dimensional Hybrid Perovskite Crystals

Jun Yin, Partha Maity, Rounak Naphade, Bin Cheng, Jr Hau He, Osman M. Bakr, Jean Luc Brédas, Omar F. Mohammed

Research output: Contribution to journalArticlepeer-review

45 Scopus citations

Abstract

Hot carrier (HC) cooling is a critical photophysical process that significantly influences the optoelectronic performance of hybrid perovskite-based devices. The hot carrier extraction at the device interface is very challenging because of its ultrashort lifetime. Here, ultrafast transient reflectance spectroscopy measurements and time-domain ab initio calculations show how the dielectric constant of the organic spacers can control and slow the HC cooling dynamics in single-crystal 2D Ruddlesden-Popper hybrid perovskites. We find that (EA)2PbI4 (EA = HOC2H4NH3 +) that correspond to a high dielectric constant organic spacer has a longer HC cooling time compared to that of (AP)2PbI4 (AP = HOC3H6NH3 +) and (PEA)2PbI4 (PEA = C6H5C2H4NH3 +). The slow HC relaxation process in the former case can be ascribed to a stronger screening of the Coulomb interactions, a small nonradiative internal conversion within the conduction bands, as well as a weak electron-phonon coupling. Our findings provide a strategy to prolong the hot carrier cooling time in low-dimensional hybrid perovskite materials by using organic spacers with reduced dielectric confinement.

Original languageEnglish (US)
Pages (from-to)12621-12629
Number of pages9
JournalACS Nano
Volume13
Issue number11
DOIs
StatePublished - Nov 26 2019
Externally publishedYes

Keywords

  • 2D hybrid perovskites
  • dielectric confinement
  • electron-phonon coupling
  • hot carrier cooling
  • nonadiabatic molecular dynamics

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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