Shear-aligned large-area organic semiconductor crystals through extended π–π interaction

Zhang, Song; Talnack, Felix; Jousselin-Oba, Tanguy; Bhat, Vinayak; Wu, Yilei; Lei, Yusheng; Tomo, Yoko; Gong, Huaxin; Michalek, Lukas; Zhong, Donglai; Wu, Can; Yassar, Abderrahim; Mannsfeld, Stefan; Risko, Chad; Frigoli, Michel; Bao, Zhenan

doi:10.1039/d3tc01311a

DOE OSTI · 2423929

Shear-aligned large-area organic semiconductor crystals through extended π–π interaction

Zhang, Song·Talnack, Felix·Jousselin-Oba, Tanguy·Bhat, Vinayak·Wu, Yilei·Lei, Yusheng·Tomo, Yoko·Gong, Huaxin·Michalek, Lukas·Zhong, Donglai·Wu, Can·Yassar, Abderrahim·Mannsfeld, Stefan·Risko, Chad·Frigoli, Michel·Bao, Zhenan

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Abstract

Small molecule-based organic semiconductors are of broad interest in organic field-effect transistors (OFETs) due to their potential for high crystallinity and electrical performance. The 2D molecule, TIPS-peri-pentacenopentacene (TIPS-PPP), which is the vertical extension of the 1D TIPS-pentacene (TIPS-PEN) molecule, offers a lower bandgap, higher aromaticity, and an enhanced π–π interaction with neighboring molecules in the solid state when compared to TIPS-PEN. However, an in-depth understanding of the relationship between the molecule structure, solid-state molecular packing, and the electronic properties has not been reported due to poor control over the TIPS-PPP crystallite size. In this work, we successfully engineered highly oriented large-area TIPS-PPP crystals through the solution shear coating technique. Additionally, compared with narrow ribbon-like TIPS-PEN crystals, TIPS-PPP crystals can grow centimeters long and over 500 μm wide. TIPS-PPP molecules are less susceptible to forming metastable polymorphs than TIPS-PEN molecules upon fast evaporation. The crystal structure of TIPS-PPP is also thermally stable at 250 °C. Notably, the anisotropic charge carrier mobility of TIPS-PPP crystals is resolved through fabricating bottom-gate top-contact devices, with a hole mobility of 3.1 cm 2 V -1 s -1 along the preferred packing direction. Further device optimization using top-gate bottom-contact devices improved the mobility up to 6.5 cm 2 V -1 s -1 , which is among the highest for pentacene-derivative-based organic semiconductors.

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Zhang, Song, Talnack, Felix, Jousselin-Oba, Tanguy, Bhat, Vinayak, Wu, Yilei, Lei, Yusheng, Tomo, Yoko, Gong, Huaxin, Michalek, Lukas, Zhong, Donglai, Wu, Can, Yassar, Abderrahim, Mannsfeld, Stefan, Risko, Chad, Frigoli, Michel, Bao, Zhenan. 2023-06-09. Shear-aligned large-area organic semiconductor crystals through extended π–π interaction. https://doi.org/10.1039/d3tc01311a

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