Ligand-Induced Surface Charge Density Modulation Generates Local Type-II Band Alignment in Reduced-Dimensional Perovskites

Journal of the American Chemical Society
Rafael Quintero-BermudezEdward H Sargent

Abstract

Two-dimensional (2D) and quasi-2D perovskite materials have enabled advances in device performance and stability relevant to a number of optoelectronic applications. However, the alignment among the bands of these variably quantum confined materials remains a controversial topic: there exist multiple experimental reports supporting type-I, and also others supporting type-II, band alignment among the reduced-dimensional grains. Here we report a combined computational and experimental study showing that variable ligand concentration on grain surfaces modulates the surface charge density among neighboring quantum wells. Density functional theory calculations and ultraviolet photoelectron spectroscopy reveal that the effective work function of a given quantum well can be varied by modulating the density of ligands at the interface. These induce type-II interfaces in otherwise type-I aligned materials. By treating 2D perovskite films, we find that the effective work function can indeed be shifted down by up to 1 eV. We corroborate the model via a suite of pump-probe transient absorption experiments: these manifest charge transfer consistent with a modulation in band alignment of at least 200 meV among neighboring grains. The finding...Continue Reading

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Sep 12, 2018·Nature Materials·Rafael Quintero-BermudezEdward H Sargent

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Citations

Feb 11, 2021·The Journal of Physical Chemistry Letters·Zhuo XuShengzhong Frank Liu
Mar 26, 2021·Journal of the American Chemical Society·Ming-Yu KuoJohn C Wright
May 7, 2020·The Journal of Physical Chemistry Letters·Rafael Quintero-BermudezRafael Quintero-Torres
Mar 12, 2020·The Journal of Physical Chemistry Letters·Junsang ChoPrashant V Kamat
Jan 7, 2020·The Journal of Physical Chemistry Letters·Ziren ZhouHua Gui Yang
Mar 30, 2020·The Journal of Physical Chemistry Letters·Linghai ZhangGang Lu
Oct 8, 2021·Advanced Materials·Junsang ChoPrashant V Kamat

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