Abstract

Optimizing the morphology of bulk heterojunctions is known to significantly improve the photovoltaic performance of organic solar cells, but available quantitative imaging techniques are few and have severe limitations. We demonstrate X-ray ptychographic coherent diffractive imaging applied to all-organic blends. Specifically, the phase-separated morphology in bulk heterojunction photoactive layers for organic solar cells, prepared from a 50:50 blend of poly(3-hexylthiophene) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) and thermally treated for different annealing times is imaged to high resolution. Moreover, using a fast-scanning calorimetry chip setup, the nano-morphological changes caused by repeated thermal annealing applied to the same sample could be monitored. X-ray ptychography resolves to better than 100 nm the phase-segregated domains of electron donor and electron acceptor materials over a large field of view within the active layers. The quantitative phase contrast images further allow us to estimate the local volume fraction of PCBM across the photovoltaically active layers. The volume fraction gradient for different regions provides insight on the PCBM diffusion across the depletion zone surrounding PCBM aggregates. Phase contrast X-ray microscopy is under rapid development, and the results presented here are promising for future studies of organic-organic blends, also under in situ conditions, e.g., for monitoring the structural stability during UV-Vis irradiation.

Highlights

  • Polymer solar cells offer a potential solution to the global energy crisis due to their cost-effectiveness, flexibility, lightweight, large-scale manufacturing characteristics, and efficient conversion of sunlight to electricity [1]

  • Solar cells based on conjugated polymers acting as electron donor materials blended with fullerene-based electron acceptor material have achieved up to 11.7% power conversion efficiency (PCE) using a single-layer bulk heterojunction (BHJ) device structure [2]

  • The sample annealed for 7500 s shows large domains, and for further analysis, we assumed that the regions in the 7500 s sample showing the largest phase shifts correspond to essentially pure phases of phenyl-C61-butyric acid methyl ester (PCBM) (P3HT) [34]

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Summary

Introduction

Polymer solar cells offer a potential solution to the global energy crisis due to their cost-effectiveness, flexibility, lightweight, large-scale manufacturing characteristics, and efficient conversion of sunlight to electricity [1]. Solar cells based on conjugated polymers acting as electron donor materials blended with fullerene-based electron acceptor material have achieved up to 11.7% power conversion efficiency (PCE) using a single-layer bulk heterojunction (BHJ) device structure [2]. Blends of poly(3-hexylthiophene) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) are a benchmark class of photovoltaically active materials [3], forming two partially miscible phases that are segregated in a random fashion. A donor and acceptor percolating network is formed, yielding a large interfacial BHJ promoting charge separation.

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