Tracking Photoexcited Carriers in Hybrid Perovskite Semiconductors: Trap-Dominated Spatial Heterogeneity and Diffusion

ACS Nano
Dane W deQuilettesDavid S Ginger

Abstract

We use correlated confocal and wide-field fluorescence microscopy to probe the interplay between local variations in charge carrier recombination and charge carrier transport in methylammonium lead triiodide perovskite thin films. We find that local photoluminescence variations present in confocal imaging are also observed in wide-field imaging, while intensity-dependent confocal measurements show that the heterogeneity in nonradiative losses observed at low excitation powers becomes less pronounced at higher excitation powers. Both confocal and wide-field images show that carriers undergo anisotropic diffusion due to differences in intergrain connectivity. These data are all qualitatively consistent with trap-dominated variations in local photoluminescence intensity and with grain boundaries that exhibit varying degrees of opacity to carrier transport. We use a two-dimensional kinetic model to simulate and compare confocal time-resolved photoluminescence decay traces with experimental data. The simulations further support the assignment of local variations in nonradiative recombination as the primary cause of photoluminescence heterogeneity in the films studied herein. These results point to surface passivation and intergrain ...Continue Reading

References

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Citations

Oct 29, 2018·Advanced Materials·Gede W P AdhyaksaErik C Garnett
Apr 10, 2019·Nature Communications·Adrien BercegolLaurent Lombez
Feb 12, 2020·Nature Materials·Makhsud I SaidaminovEdward H Sargent
Feb 5, 2019·Energy & Environmental Science·Camille StavrakasSamuel D Stranks
Jun 9, 2021·Nature Communications·Alexander KiligaridisIvan G Scheblykin
Jun 9, 2018·The Journal of Physical Chemistry Letters·John M HowardMarina S Leite
Sep 10, 2019·Chemical Reviews·Dane W deQuilettesSamuel D Stranks
Aug 14, 2019·The Journal of Physical Chemistry Letters·Dibyajyoti GhoshAmanda J Neukirch
Aug 14, 2020·Chemical Reviews·Jin Young KimNam-Gyu Park
Feb 15, 2020·ACS Energy Letters·Camille StavrakasSamuel D Stranks
Feb 18, 2020·Chemistry of Materials : a Publication of the American Chemical Society·Dibyajyoti GhoshM Saiful Islam
Aug 28, 2020·Journal of the American Chemical Society·Ti WangLibai Huang

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