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Close-Packed Ultrasmooth Self-assembled Monolayer of CsPbBr3 Perovskite Nanocubes.

ABSTRACT: The use of colloidal self-assembly to form the complex multiscale patterns in many optoelectronic devices has been a long-standing dream of the nanoscience community. While great progress has been made using charged colloids in polar solvents, controlled assembly from nonpolar solvents is much more challenging. The major challenge is colloidal clustering caused by strong van der Waals (vdW) attraction between long-chain surface capping ligands passivating the surface of nanocrystals. Such clustering degrades ordering in packing during the self-assembly process. While ligand exchange to provide colloidal stability in polar phases is often an option, this is not the case for the exciting new class of halide perovskites due to the material's solubility in essentially all polar solvents. Here, we report surface-functionalized self-assembly of luminescent CsPbBr3 perovskite nanocubes by partially replacing long-chain oleyl groups (18 carbon chain) with short-chain thiocyanate (SCN-). This enables the fabrication of ultrasmooth monolayer thin films of nanocubes with a root-mean-square (RMS) roughness of around 4 Å. This ultrasmooth large area self-assembled layer could act as high-efficiency optoelectronic devices like solar cells, light-emitting diodes (LEDs), transistors, etc. We correlate our experimental results with simulations, providing detailed predictions for lattice constants with chain conformations showing reduced free energy for cubes grafted with short-chain thiocyanate compared to long-chain oleyl groups, thus facilitating better self-assembly.

SUBMITTER: Patra BK

PROVIDER: S-EPMC7430943 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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Close-Packed Ultrasmooth Self-assembled Monolayer of CsPbBr<sub>3</sub> Perovskite Nanocubes.

Patra Biplab K BK Agrawal Harshal H Zheng Jian-Yao JY Zha Xun X Travesset Alex A Garnett Erik C EC

ACS applied materials & interfaces 20200630 28

The use of colloidal self-assembly to form the complex multiscale patterns in many optoelectronic devices has been a long-standing dream of the nanoscience community. While great progress has been made using charged colloids in polar solvents, controlled assembly from nonpolar solvents is much more challenging. The major challenge is colloidal clustering caused by strong van der Waals (vdW) attraction between long-chain surface capping ligands passivating the surface of nanocrystals. Such cluste ...[more]

PMID: 32545949

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Project description:Metal halide perovskites have attracted tremendous attention due to their excellent electronic properties. Recent advancements in device performance and stability of perovskite solar cells (PSCs) have been achieved with the application of self-assembled monolayers (SAMs), serving as stand-alone hole transport layers in the p-i-n architecture. Specifically, phosphonic acid SAMs, directly functionalizing indium-tin oxide (ITO), are presently adopted for highly efficient devices. Despite their successes, so far, little is known about the surface coverage of SAMs on ITO used in PSCs application, which can affect the device performance, as non-covered areas can result in shunting or low open-circuit voltage. In this study, we investigate the surface coverage of SAMs on ITO and observe that the SAM of MeO-2PACz ([2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid) inhomogeneously covers the ITO substrate. Instead, when adopting an intermediate layer of NiO between ITO and the SAM, the homogeneity, and hence the surface coverage of the SAM, improve. In this work, NiO is processed by plasma-assisted atomic layer deposition (ALD) with Ni(MeCp)2 as the precursor and O2 plasma as the co-reactant. Specifically, the presence of ALD NiO leads to a homogeneous distribution of SAM molecules on the metal oxide area, accompanied by a high shunt resistance in the devices with respect to those with SAM directly processed on ITO. At the same time, the SAM is key to the improvement of the open-circuit voltage of NiO + MeO-2PACz devices compared to those with NiO alone. Thus, the combination of NiO and SAM results in a narrower distribution of device performance reaching a more than 20% efficient champion device. The enhancement of SAM coverage in the presence of NiO is corroborated by several characterization techniques including advanced imaging by transmission electron microscopy (TEM), elemental composition quantification by Rutherford backscattering spectrometry (RBS), and conductive atomic force microscopy (c-AFM) mapping. We believe this finding will further promote the usage of phosphonic acid based SAM molecules in perovskite PV.

Dataset Information

Close-Packed Ultrasmooth Self-assembled Monolayer of CsPbBr3 Perovskite Nanocubes.

Publications

Close-Packed Ultrasmooth Self-assembled Monolayer of CsPbBr<sub>3</sub> Perovskite Nanocubes.

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