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Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS.

ABSTRACT: Extensive attention has focused on the structure optimization of perovskites, whereas rare research has mapped the structure heterogeneity within mixed hybrid perovskite films. Overlooked aspects include material and structure variations as a function of depth. These depth-dependent local structure heterogeneities dictate their long-term stabilities and efficiencies. Here, we use a nano-focused wide-angle X-ray scattering method for the mapping of film heterogeneities over several micrometers across lateral and vertical directions. The relative variations of characteristic perovskite peak positions show that the top film region bears the tensile strain. Through a texture orientation map of the perovskite (100) peak, we find that the perovskite grains deposited by sequential spray-coating grow along the vertical direction. Moreover, we investigate the moisture-induced degradation products in the perovskite film, and the underlying mechanism for its structure-dependent degradation. The moisture degradation along the lateral direction primarily initiates at the perovskite-air interface and grain boundaries. The tensile strain on the top surface has a profound influence on the moisture degradation.

SUBMITTER: Li N

PROVIDER: S-EPMC9637205 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature

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Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS.

Li Nian N Pratap Shambhavi S Körstgens Volker V Vema Sundeep S Song Lin L Liang Suzhe S Davydok Anton A Krywka Christina C Müller-Buschbaum Peter P

Nature communications 20221105 1

Extensive attention has focused on the structure optimization of perovskites, whereas rare research has mapped the structure heterogeneity within mixed hybrid perovskite films. Overlooked aspects include material and structure variations as a function of depth. These depth-dependent local structure heterogeneities dictate their long-term stabilities and efficiencies. Here, we use a nano-focused wide-angle X-ray scattering method for the mapping of film heterogeneities over several micrometers ac ...[more]

PMID: 36335119

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Project description:Organic-inorganic halide perovskites are interesting candidates for solar cell and optoelectronic applications owing to their advantageous properties such as a tunable band gap, low material cost, and high charge carrier mobilities. Despite making significant progress, concerns about material stability continue to impede the commercialization of perovskite-based technology. In this article, we investigate the impact of environmental parameters on the alteration of structural properties of MAPbI3 (CH3NH3PbI3) thin films using microscopy techniques. These characterizations are performed on MAPbI3 thin films exposed to air, nitrogen, and vacuum environments, the latter being possible by using dedicated air-free transfer setups, after their fabrication into a nitrogen-filled glovebox. We observed that even less than 3 min of air exposure increases the sensitivity to electron beam deterioration and modifies the structural transformation pathway as compared to MAPbI3 thin films which are not exposed to air. Similarly, the time evolution of the optical responses and the defect formation of both air-exposed and non-air-exposed MAPbI3 thin films are measured by time-resolved photoluminescence. The formation of defects in the air-exposed MAPbI3 thin films is first observed by optical techniques at longer timescales, while structural modifications are observed by transmission electron microscopy (TEM) measurements and supported by X-ray photoelectron spectroscopy (XPS) measurements. Based on the complementarity of TEM, XPS, and time-resolved optical measurements, we propose two different degradation mechanism pathways for air-exposed and non-air-exposed MAPbI3 thin films. We find that when exposed to air, the crystalline structure of MAPbI3 shows gradual evolution from its initial tetragonal MAPbI3 structure to PbI2 through three different stages. No significant structural changes over time from the initial structure are observed for the MAPbI3 thin films which are not exposed to air.

Dataset Information

Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS.

Publications

Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS.

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