Browsing by Author "Shivhare, Rishi"
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- ItemHighly Crystalline and Semiconducting Imine-Based Two-Dimensional Polymers Enabled by Interfacial Synthesis(Weinheim : Wiley-VCH, 2020) Sahabudeen, Hafeesudeen; Qi, Haoyuan; Ballabio, Marco; Položij, Miroslav; Olthof, Selina; Shivhare, Rishi; Jing, Yu; Park, SangWook; Liu, Kejun; Zhang, Tao; Ma, Ji; Rellinghaus, Bernd; Mannsfeld, Stefan; Heine, Thomas; Bonn, Mischa; Cánovas, Enrique; Zheng, Zhikun; Kaiser, Ute; Dong, Renhao; Feng, XinliangSingle-layer and multi-layer 2D polyimine films have been achieved through interfacial synthesis methods. However, it remains a great challenge to achieve the maximum degree of crystallinity in the 2D polyimines, which largely limits the long-range transport properties. Here we employ a surfactant-monolayer-assisted interfacial synthesis (SMAIS) method for the successful preparation of porphyrin and triazine containing polyimine-based 2D polymer (PI-2DP) films with square and hexagonal lattices, respectively. The synthetic PI-2DP films are featured with polycrystalline multilayers with tunable thickness from 6 to 200 nm and large crystalline domains (100–150 nm in size). Intrigued by high crystallinity and the presence of electroactive porphyrin moieties, the optoelectronic properties of PI-2DP are investigated by time-resolved terahertz spectroscopy. Typically, the porphyrin-based PI-2DP 1 film exhibits a p-type semiconductor behavior with a band gap of 1.38 eV and hole mobility as high as 0.01 cm2 V−1 s−1, superior to the previously reported polyimine based materials. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemInvestigating the morphology of bulk heterojunctions by laser photoemission electron microscopy(Amsterdam [u.a.] : Elsevier Science, 2022) Niefind, Falk; Shivhare, Rishi; Mannsfeld, Stefan C.B.; Abel, Bernd; Hambsch, MikeThe nanoscale morphology of bulk heterojunctions is highly important for the charge dissociation and transport in organic solar cells and ultimately defines the performance of the cell. The visualization of this nano-morphology in terms of domain size and polymer orientation in a fast and straightforward way is therefore of great interest to evaluate the suitability of a film for efficient solar cells. Here, we demonstrate that the morphology of different blends of poly(3-hexylthiophene-2,5-diyl) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) can be imaged and analyzed by employing photoemission electron microscopy.
- ItemShort Excited-State Lifetimes Mediate Charge-Recombination Losses in Organic Solar Cell Blends with Low Charge-Transfer Driving Force(Weinheim : Wiley-VCH, 2021) Shivhare, Rishi; Moore, Gareth John; Hofacker, Andreas; Hutsch, Sebastian; Zhong, Yufei; Hambsch, Mike; Erdmann, Tim; Kiriy, Anton; Mannsfeld, Stefan C.B.; Ortmann, Frank; Banerji, NatalieA blend of a low-optical-gap diketopyrrolopyrrole polymer and a fullerene derivative, with near-zero driving force for electron transfer, is investigated. Using femtosecond transient absorption and electroabsorption spectroscopy, the charge transfer (CT) and recombination dynamics as well as the early-time transport are quantified. Electron transfer is ultrafast, consistent with a Marcus-Levich-Jortner description. However, significant charge recombination and unusually short excited (S1 ) and CT state lifetimes (≈14 ps) are observed. At low S1 -CT offset, a short S1 lifetime mediates charge recombination because: i) back-transfer from the CT to the S1 state followed by S1 recombination occurs and ii) additional S1 -CT hybridization decreases the CT lifetime. Both effects are confirmed by density functional theory calculations. In addition, relatively slow (tens of picoseconds) dissociation of charges from the CT state is observed, due to low local charge mobility. Simulations using a four-state kinetic model entailing the effects of energetic disorder reveal that the free charge yield can be increased from the observed 12% to 60% by increasing the S1 and CT lifetimes to 150 ps. Alternatively, decreasing the interfacial CT state disorder while increasing bulk disorder of free charges enhances the yield to 65% in spite of the short lifetimes.