Confinement and Exciton Binding Energy Effects on Hot Carrier Cooling in Lead Halide Perovskite Nanomaterials

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

Abstract

The relaxation of the above-gap (“hot”) carriers in lead halide perovskites (LHPs) is important for applications in photovoltaics and offers insights into carrier-carrier and carrier-phonon interactions. However, the role of quantum confinement in the hot carrier dynamics of nanosystems is still disputed. Here, we devise a single approach, ultrafast pump-push-probe spectroscopy, to study carrier cooling in six different size-controlled LHP nanomaterials. In cuboidal nanocrystals, we observe only a weak size effect on the cooling dynamics. In contrast, two-dimensional systems show suppression of the hot phonon bottleneck effect common in bulk perovskites. The proposed kinetic model describes the intrinsic and density-dependent cooling times accurately in all studied perovskite systems using only carrier-carrier, carrier-phonon, and excitonic coupling constants. This highlights the impact of exciton formation on carrier cooling and promotes dimensional confinement as a tool for engineering carrier-phonon and carrier-carrier interactions in LHP optoelectronic materials.

Details

OriginalspracheEnglisch
Seiten (von - bis)6638-6648
Seitenumfang11
FachzeitschriftACS nano
Jahrgang17
Ausgabenummer7
PublikationsstatusVeröffentlicht - 11 Apr. 2023
Peer-Review-StatusJa

Externe IDs

PubMed 36939330
WOS 000962222000001

Schlagworte

Fächergruppen, Lehr- und Forschungsbereiche, Fachgebiete nach Destatis

Ziele für nachhaltige Entwicklung

Schlagwörter

  • hot carriers, nanocrystals, nanoplatelets, two-dimensional perovskites, ultrafast spectroscopy, Nanoplatelets, Nanocrystals, Two-dimensional perovskites, Hot carriers, Ultrafast spectroscopy