Abstract

Single-crystal semiconductors have been at the forefront of scientific interest for more than 70 years, serving as the backbone of electronic devices. Inorganic single crystals are typically grown from a melt using time-consuming and energy-intensive processes. Organic semiconductor single crystals, however, can be grown using solution-based methods at room temperature in air, opening up the possibility of large-scale production of inexpensive electronics targeting applications ranging from field-effect transistors and light-emitting diodes to medical X-ray detectors. Here we demonstrate a low-cost, scalable spray-printing process to fabricate high-quality organic single crystals, based on various semiconducting small molecules on virtually any substrate by combining the advantages of antisolvent crystallization and solution shearing. The crystals' size, shape and orientation are controlled by the sheer force generated by the spray droplets' impact onto the antisolvent's surface. This method demonstrates the feasibility of a spray-on single-crystal organic electronics.

Highlights

  • Single-crystal semiconductors have been at the forefront of scientific interest for more than 70 years, serving as the backbone of electronic devices

  • The progress in modern electronics in the last seven decades was closely linked with the development of singlecrystalline semiconducting materials, initially represented by silicon and germanium[1], and recently enriched by a new class of organic semiconducting single crystals (OSSCs)[2,3,4,5,6], offering enhanced physical properties demonstrated in light-emitting transistors[7] and human tissue equivalent materials for medical X-ray detectors[8]

  • Significant improvements have been demonstrated in the performance of field-effect transistors (FETs) by using this approach, the active layer still retains its polycrystalline nature, which is unfavourable for applications such as lasing[17] and highenergy isotope detection[18,19]

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Summary

Introduction

Single-crystal semiconductors have been at the forefront of scientific interest for more than 70 years, serving as the backbone of electronic devices. Can be grown using solution-based methods at room temperature in air, opening up the possibility of large-scale production of inexpensive electronics targeting applications ranging from field-effect transistors and light-emitting diodes to medical X-ray detectors. Significant improvements have been demonstrated in the performance of field-effect transistors (FETs) by using this approach, the active layer still retains its polycrystalline nature, which is unfavourable for applications such as lasing[17] and highenergy isotope detection[18,19] These applications require highly ordered single crystals with well-defined boundaries. The solution shearing technique addressed the issue of one-step patterned crystallization and in some cases produced remarkable results for the charge carrier properties in FETs20 Such processes still lead to polycrystalline semiconducting films, making the approach incompatible with a broad range of applications. The single-crystalline nature of the crystals has been examined by a combination of techniques probing both local molecular orientation and order with X-ray diffraction (XRD) and polarized Raman, and evaluating the overall large area uniformity of the crystals with polarized optical and scanning electron microscopy (SEM)

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