Journal
MATERIALS HORIZONS
Volume 6, Issue 9, Pages 1868-1876Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9mh00035f
Keywords
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Funding
- United States Army Research Office [W911NF-15-1-0447]
- National Science Foundation Graduate Research Fellowship [DGE-1324585]
- Ryan Fellowship
- Northwestern University International Institute for Nanotechnology
- National Science Foundation [DMR-1708147]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1720139]
- Keck Foundation
- State of Illinois
- International Institute for Nanotechnology (IIN)
- U.S. Department of Energy (DOE) [DE-AC36-08GO28308]
- Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences
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We have considered three two-dimensional (2D) pi-conjugated polymer network (i.e., covalent organic frameworks, COFs) materials based on pyrene, porphyrin, and zinc-porphyrin cores connected via diacetylenic linkers. Their electronic structures, investigated at the density functional theory global-hybrid level, are indicative of valence and conduction bands that have large widths, ranging between 1 and 2 eV. Using a molecular approach to derive the electronic couplings between adjacent core units and the electron-vibration couplings, the three pi-conjugated 2D COFs are predicted to have ambipolar charge-transport characteristics with electron and hole mobilities in the range of 65-95 cm(2) V-1 s(-1). Such predicted values rank these 2D COFs among the highest-mobility organic semiconductors. In addition, we have synthesized the zinc-porphyrin based 2D COF and carried out structural characterization via powder X-ray diffraction, high-resolution transmission electron microscopy, and surface area analysis, which demonstrates the feasibility of these electroactive networks. Steady-state and flash-photolysis time-resolved microwave conductivity measurements on the zinc-porphyrin COF point to appreciable, broadband photoconductivity while transmission spectral measurements are indicative of extended pi-conjugation.
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