Molecularly Thin 2D Organic Single Crystals: A New Platform for High-Performance Polarization-Sensitive Phototransistors.

The inherent linear dichroism (LD), high absorption, and solution processability of organic semiconductors hold immense potential to revolutionize polarized light detection. However, the disordered molecular packing inherent to polycrystalline thin films obscures their intrinsic diattenuation, resulting in diminished polarization sensitivity. In this study, we develop filter-free organic polarization-sensitive phototransistors (PSPs) with both a high linear dichroic ratio (LDR) and exceptional photosensitivity utilizing molecularly thin dithieno[3,2-b:2',3'-d]thiophene derivatives (DTT-8) two-dimensional molecular crystals (2DMCs) as the active layer. The orderly molecular packing in 2DMCs amplifies the inherent LD, and their molecular-scale thickness enables complete channel depletion, significantly reducing the dark current. As a result, PSPs with an impressive LDR of 3.15 and a photosensitivity reaching 3.02 × 106 are obtained. These findings present a practical demonstration of using the polarization angle as an encryption key in optical communication, showcasing the potential of 2DMCs as a viable and promising category of semiconductors for filter-free, polarization-sensitive photodetectors.

Thermal-assisted self-assembly: a self-adaptive strategy towards large-area uniaxial organic single-crystalline microribbon arrays.

Uniaxial organic single-crystalline microribbon arrays (OSCMAs) are a class of highly desirable materials for a variety of optoelectronic applications due to their favorable molecular orientations along the long axes of the ribbons. Up to now, great endeavors have been made and several solution-processing techniques have been proposed to grow uniaxial OSCMAs. However, the crystal growth parameters are tuned non-synergistically in these techniques, resulting in challenging growth condition control. Herein, we report a self-adaptive thermal-assisted self-assembly (TASA) strategy to realize the synergistic control of key crystal growth parameters for the facile yet controllable production of centimeter-sized uniaxial OSCMAs from the solution. In the TASA strategy, key crystal growth parameters, such as solvent evaporation, nucleation and crystal growth, are controlled synergistically by the temperature gradient. As a result, the TASA strategy is self-adaptive, and it shows a large temperature and concentration tolerance. Organic phototransistors (OPTs) based on the uniaxial OSCMAs produced by the TASA strategy exhibit an unprecedented photosensitivity of 1.36 × 108, a high responsivity of 845 A W-1 and a high detectivity of 1.98 × 1015 Jones.