Journal
ADVANCED MATERIALS
Volume 30, Issue 38, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201803467
Keywords
charge transport; electron mobility; organic field-effect transistors; organic semiconductors
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Funding
- Research Grants Council of Hong Kong [GRF 14300217]
- University Grants Committee of Hong Kong [AoE/P-03/08]
- Ministry of Science and Technology of China [2017YFA0204503]
- National Natural Science Foundation of China [51725304, 21473071]
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Molecular engineering of tetraazapentacene with different numbers of fluorine and chlorine substituents fine-tunes the frontier molecular orbitals, molecular vibrations, and pi-pi stacking for n-type organic semiconductors. Among the six halogenated tetraazapentacenes studied herein, the tetrachloro derivative (4Cl-TAP) in solution-processed thin-film transistors exhibits electron mobility of 14.9 +/- 4.9 cm(2) V-1 s(-1) with a maximum value of 27.8 cm(2) V-1 s(-1), which sets a new record for n-channel organic field-effect transistors. Computational studies on the basis of crystal structures shed light on the structure-property relationships for organic semiconductors. First, chlorine substituents slightly decrease the reorganization energy of the tetraazapentacene whereas fluorine substituents increase the reorganization energy as a result of fine-tuning molecular vibrations. Second, the electron transfer integral is very sensitive to subtle changes in the 2D pi-stacking with brickwork arrangement. The unprecedentedly high electron mobility of 4Cl-TAP is attributed to the reduced reorganization energy and enhanced electron transfer integral as a result of modification of tetraazapentacene with four chlorine substituents.
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