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We develop theoretical descriptions for charge transport in organic semiconductors and carbon nanomaterials. For the localized charges, we found the quantum nuclear tunneling effect is essential which could manifest isotope effect for mobility as well as exotic optical feature. Because the nuclear tunneling tends to favor electron transfer while heavier nuclei decrease the quantum effect, isotopic substitution should reduce carrier mobility. Moreover, the isotopic effect only occurs when the substituted nuclei contribute actively to vibrations with appreciable charge reorganization energy and coupling with carrier motion. For the band-like transport, we propose a Wannier extrapolation scheme for computing the electron-phonon interaction matrix for the Boltzmann equation. Our calculation indicates that the intrinsic electron-phonon scatterings in two-dimensional carbon materials are dominated by low-energy longitudinal-acoustic phonon scatterings over a wide range of temperatures, while by high-frequency optical phonons at high temperature. The electron mobilities of α- and γ-graphynes are predicted to be ca.104 cm2V-1s-1 at room temperature.
We present a comparative study of optical absorption, photoluminescence (PL), and photoconductivity in bulk heterojunctions comprising a high performance functionalized anthradithiophene (ADT) derivative or the benchmark polymer P3HT as donor and functionalized pentacene (Pn) derivative or PCBM as acceptor. Of all D/A blends studied, the ADT/PCBM blend exhibited the highest charge photogeneration efficiencies under 532 nm excitation, leading to the highest amplitudes of time-resolved and continuous wave (cw) photocurrents. At nanosecond time scales after photoexcitation, both ADT-TES-F-based blends and the P3HT/Pn-TIPS-F8 blend exhibited photocurrents which were higher by a factor of 2-10, depending on the blend, than that in the P3HT/PCBM blend. However, cw photocurrents showed a different trend, with the ADT-TES-F/PCBM blend exhibiting only a factor of ∼2.5 higher photoresponse than that in the P3HT/PCBM blends, and the ADT-TES-F- and P3HT- based blends with Pn-TIPS-F8 showing a factor of ∼1.5-2.5 lower photoresponse than that in the P3HT/PCBM blend, due to other contributions, such as that of charge trap-limited transport, to cw photoresponse.
Core substituted perylene diimides (PDIs) are promising candidates as non-fullerene acceptor materials for organic solar cells. The functionalization of PDIs in the bay positions using chemical groups with different electron donating abilities and with steric hindrance is a versatile tool to modify both the optoelectronic properties and the morphology in the solid state.
Herein we present two new PDI based molecules having bulky aromatic substituents linked into the bay positions: PDI-SF with spirobifluorene group and PDI-BSF with bithienyl-spirobifluorene moieties. The high steric hindrance of spirobifluorene reduce the tendency to form aggregates that has been identified as a limiting factor for the photovoltaic performances in PDI based solar cells.
The PDI molecules were tested as electron acceptors in bulk heterojunction solar cells with P3HT as electron donor. Power conversion efficiencies (PCE) of 1.58% and 1.18% were obtained for PDI-SF and PDI-BSF devices.
Poly (3-hexylthiophene) (P3HT) thin films were deposited using emulsion-based, resonant infrared matrix-assisted pulsed laser evaporation (RIR-MAPLE) from emulsions containing different solvents and different alcohols, to investigate the impact of emulsion on film morphology. The atomic force microscopy (AFM) and grazing-incidence, wide angle x-ray scattering (GIWAXS) results show that surface morphology of RIR-MAPLE as-deposited films can be varied from rough to smooth and the microcrystalline domain orientations with respect to the substrate can be tuned from randomly oriented to preferentially oriented in the vertical direction. The demonstrated ability to tune the structural characteristics of polymer thin films by controlling the target emulsion is important for the application of organic optoelectronic devices deposited by RIR-MAPLE.