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Abstract
Molecular self-assembly into crystallised films or wires on surfaces produces a big family of motifs exhibiting unique optoelectronic properties. However, little attention has been paid to the fundamental mechanism of molecular crystallisation. Here we report a biomimetic design of phosphonate engineered, amphiphilic organic semiconductors capable of self–assembly, which enables us to use real-time in-situ scanning probe microscopy to monitor the growth trajectories of such organic semiconducting films as they nucleate and crystallise from amorphous solid states. The single-crystal film grows through an evolutionary selection approach in a two-dimensional geometry, with five distinct steps: droplet flattening, film coalescence, spinodal decomposition, Ostwald ripening, and self-reorganised layer growth. These sophisticated processes afford ultralong high-density microwire arrays with high mobilities, thus promoting deep understanding of the mechanism as well as offering important insights into the design and development of functional high-performance organic optoelectronic materials and devices through molecular and crystal engineering.
Highlights
Molecular self-assembly into crystallised films or wires on surfaces produces a big family of motifs exhibiting unique optoelectronic properties
Molecular engineering has enabled synthetic chemists to mimic liquid crystalline structures through the self-assembly of predesigned molecules from their anisotropic amorphous states[5,6,7], yet little attention has been given to the fundamental mechanism by which they nucleate on the surfaces
Inspired by the fact that the inherent chemical structure duality and the hydrophobic effect enable phospholipids to self-aggregate into a lamellar bilayer structure, we demonstrate in this study a series of phosphonate engineered, amphiphilic organic semiconductors (OSCs) that can grow via a process termed as crystallisation-driven self-assembly (CDSA)[17,18,19] to form ultralong, high-density and highly ordered microwire arrays
Summary
Molecular self-assembly into crystallised films or wires on surfaces produces a big family of motifs exhibiting unique optoelectronic properties. Inspired by the fact that the inherent chemical structure duality and the hydrophobic effect enable phospholipids to self-aggregate into a lamellar bilayer structure, we demonstrate in this study a series of phosphonate engineered, amphiphilic organic semiconductors (OSCs) that can grow via a process termed as crystallisation-driven self-assembly (CDSA)[17,18,19] to form ultralong, high-density and highly ordered microwire arrays By integrating this molecular design with real-time in situ atomic force microscopy (AFM) and film X-ray diffraction (XRD), we successfully imaged the entire self-assembly trajectories and the kinetics of the crystallised films at the minute timescale under ambient conditions
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