Electron-Hole Binding Governs Carrier Transport in Halide Perovskite Nanocrystal Thin Films.

Autor: Lichtenegger MF; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Drewniok J; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Bornschlegl A; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Lampe C; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Singldinger A; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Henke NA; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany., Urban AS; Nanospectroscopy Group and Center for Nanoscience (CeNS), Nano-Institute Munich, Department of Physics, Ludwig-Maximiliäns-Universitat München, Königinstr. 10, 80539 Munich, Germany.
Jazyk: angličtina
Zdroj: ACS nano [ACS Nano] 2022 Apr 26; Vol. 16 (4), pp. 6317-6324. Date of Electronic Publication: 2022 Mar 18.
DOI: 10.1021/acsnano.2c00369
Abstrakt: Two-dimensional halide perovskite nanoplatelets (NPLs) have exceptional light-emitting properties, including wide spectral tunability, ultrafast radiative decays, high quantum yields (QY), and oriented emission. Due to the high binding energies of electron-hole pairs, excitons are generally considered the dominant species responsible for carrier transfer in NPL films. To realize efficient devices, it is imperative to understand how exciton transport progresses therein. We employ spatially and temporally resolved optical microscopy to map exciton diffusion in perovskite nanocrystal (NC) thin films between 15 °C and 55 °C. At room temperature (RT), we find the diffusion length to be inversely correlated to the thickness of the nanocrystals (NCs). With increasing temperatures, exciton diffusion declines for all NC films, but at different rates. This leads to specific temperature turnover points, at which thinner NPLs exhibit higher diffusion lengths. We attribute this anomalous diffusion behavior to the coexistence of excitons and free electron hole-pairs inside the individual NCs within our temperature range. The organic ligand shell surrounding the NCs prevents charge transfer. Accordingly, any time an electron-hole pair spends in the unbound state reduces the FRET-mediated inter-NC transfer rates and, consequently, the overall diffusion. These results clarify how exciton diffusion progresses in strongly confined halide perovskite NC films, emphasizing critical considerations for optoelectronic devices.
Databáze: MEDLINE