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Band-like transport in small-molecule thin films toward high mobility and ultrahigh detectivity phototransistor arrays.

ABSTRACT: With the fast development of organic electronics, organic semiconductors have been extensively studied for various optoelectronic applications, among which organic phototransistors recently emerged as one of the most promising light signal detectors. However, it is still a big challenge to endow organic phototransistors with both high mobility and high light-sensitivity because the low mobility of most organic photoresponsive materials limits the efficiency of transporting and collecting charge carriers. We herein report band-like charge transport in vacuum-deposited small-molecule thin films for organic phototransistor arrays which can be operated at very low dark currents (~10^-12?A). Both high mobility and excellent optical figures of merit including photosensitivity, photoresponsivity and detectivity are achieved, wherein, unprecedentedly, a detectivity greater than 10¹⁷?cm?Hz^1/2?W^-1 is obtained. All these key parameters are superior to state-of-the-art organic phototransistors, implying a great potential in optoelectronic applications.

SUBMITTER: Ji D

PROVIDER: S-EPMC6315033 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Band-like transport in small-molecule thin films toward high mobility and ultrahigh detectivity phototransistor arrays.

Ji Deyang D Li Tao T Liu Jie J Amirjalayer Saeed S Zhong Mianzeng M Zhang Zhao-Yang ZY Huang Xianhui X Wei Zhongming Z Dong Huanli H Hu Wenping W Fuchs Harald H

Nature communications 20190102 1

With the fast development of organic electronics, organic semiconductors have been extensively studied for various optoelectronic applications, among which organic phototransistors recently emerged as one of the most promising light signal detectors. However, it is still a big challenge to endow organic phototransistors with both high mobility and high light-sensitivity because the low mobility of most organic photoresponsive materials limits the efficiency of transporting and collecting charge ...[more]

PMID: 30602727

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Project description:ConspectusThe crystal structure of organic semiconductors has been regarded as one of the crucial factors for realizing high-performance electronic devices, such as organic field-effect transistors. However, although the control of crystal structures of organic semiconductors has been examined in the last two decades of intensive efforts of the development of organic semiconductors, active measures to control crystal structures enabling high carrier mobility are still limited. In 2016, our research group noticed that regioselective methylthiolation could provide a selective crystal structure change from an ordinary herringbone structure to a pitched π-stacking structure, similar to the crystal structure of rubrene, in the benzo[1,2-b:4,5-b']dithiophene (BDT) system. Following this serendipitous finding, our group systematically investigated the relationship between the molecular and crystal structures of a range of methylthiolated aromatic and heteroaromatic compounds.This Account provides a comprehensive overview of our research efforts and advancements in the development of methylthiolated small-molecule-based organic semiconductors (molecular semiconductors). We first describe the outline of the past development of molecular semiconductors, focusing on the types of crystal structures of high-performance molecular semiconductors. Then, we describe our findings on the drastic crystal structure change in the BDT system upon methylthiolation, detailing the causes of the change in terms of the intermolecular contacts and intermolecular interaction energies. This is followed by the confirmation of the generality of the crystal-structure change by methylthiolation of a series of acene and heteroacenes, where the herringbone structure in the parent system is unexceptionally transformed into the pitched π-stacking structure, a promising crystal structure for high-mobility molecular semiconductors well exemplified by the prototypical molecular semiconductor, rubrene. In fact, the methylthiolated anthradithiophene afforded comparable high mobility to rubrene in single-crystal field-effect transistors. Then, we demonstrate that the sandwich herringbone structures of peri-condensed polycyclic aromatic hydrocarbons, including pyrene, perylene, and peropyrene, change into brickwork crystal structures upon methylthiolation and that, among these compounds, very promising molecular semiconductors, methylthiolated pyrene and peropyrene, showing ultrahigh mobility of 30 cm2 V s-1, are realized.Through the studies, by gaining insights into the underlying mechanisms driving the crystal structure changes, we lay a strong foundation for tackling challenges related to controlling the crystal structures and developing high-performance molecular semiconductors. This will be a distinct approach from the past activities in the development of molecular semiconductors that mainly focused on molecules themselves, including their synthesis, properties, and characterization. We thus anticipate that our findings and the present Account will open the door to a new era of the development of molecular semiconductors.

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Band-like transport in small-molecule thin films toward high mobility and ultrahigh detectivity phototransistor arrays.

Publications

Band-like transport in small-molecule thin films toward high mobility and ultrahigh detectivity phototransistor arrays.

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