Through the use of photoelectron spectroscopy in air (PESA), we investigate the size-dependent valence and conduction band-edge energies of CdSe, CdTe, PbS, and PbSe semiconductor quantum dots (QDs). The results are compared to those of previous studies, based on differing experimental methods, and to theoretical calculations based on k·p theory and state-of-the-art atomistic semiempirical pseudopotential modeling. To accurately map out the energy level landscapes of QDs as a function of size, the QDs must be passivated by comparable surface chemistries. This is highlighted by studying the effect of surface chemistry on the valence band-edge energy in an ensemble of 4.7 nm CdSe QDs. An energy level shift as large as 0.35 eV is observed for this system through modification of surface chemistry alone. This shift is significantly larger than the size-dependent valence band-edge shift that is observed when comparable surface chemistries are used.
Fully printed perovskite solar cells are demonstrated with slot-die coating, a scalable printing method. A sequential slot-die coating process is developed to produce efficient perovskite solar cells and to be used in a large-scale roll-to-roll printing process. All layers excluding the electrodes are printed and devices demonstrate up to 11.96% power conversion efficiency. It is also demonstrated that the new process can be used in roll-to-roll production.
ABSTRACT:We report the synthesis and polymerization of a novel thieno[3,2-b]thiophene-diketopyrrolopyrrolebased monomer. Copolymerization with thiophene afforded a polymer with a maximum hole mobility of 1.95 cm 2 V -1 s -1 , which is the highest mobility from a polymer-based OFET reported to date. Bulk-heterojunction solar cells comprising this polymer and PC 71 BM gave a power conversion efficiency of 5.4%. T here is considerable interest in the synthesis of narrow-bandgap conjugated polymers for use in organic photovoltaic (OPV) and organic field-effect transistor (OFET) devices. Their solution processability and mechanical properties allow access to a new generation of cheap and flexible transistors and solar devices. Current state of the art polymeric materials have allowed for the fabrication of OFETs with mobilities of ∼1 cm 2 V -1 s -1 1 and OPV devices with power conversion efficiencies (PCEs) of over 7%.2 Diketopyrrolopyrrole (DPP)-based copolymers have emerged as extremely attractive materials for both thin-film transistors and solar cell devices in recent years. The DPP core's electrondeficient nature has been exploited for the synthesis of extremely narrow band gap donor-acceptor-type materials that are wellsuited for use in OPVs with high PCEs reported from both small molecules and polymers.3-6 Furthermore, the planarity of the DPP skeleton and its ability to accept hydrogen bonds (and other types of electrostatic interactions) result in copolymers that encourage π-π stacking. Typically, these DPP-based copolymers are prepared via either Suzuki or Stille coupling of the 3,6-bis(5-bromothiophen-2-yl)-2,5-dialkylpyrrolo[3,4-c]pyrrole-1,4-(2H,5H)-dione core with the desired comonomer, which as a result means that the electron-deficient DPP unit is always flanked by two thiophenes. Variation of the comonomer has yielded polymers with extremely attractive properties for both OPV and OFET devices. For instance, copolymerization with thiophene derivatives or benzothiadiazole resulted in polymers with impressive ambipolar charge-carrier mobilities. 7,8 Recently, a copolymer of 3,6-bis(5-bromothiophen-2-yl)-N,N 0 -bis(2-octyl-1-dodecyl)-1,4-dioxopyrrolo[3,4-c]pyrrole and 2,5-bis(trimethylstannyl)thieno[3,2-b]thiophene showed an impressive hole mobility of ∼0.9 cm 2 V -1 s -1 . 9 In terms of materials for OPVs, copolymerization of the same DPP monomer (albeit having a slightly different solubilizing alkyl chain) with phenylene-1,4-diboronic acid bispinacol ester afforded a polymer that was used to fabricate OPV devices with efficiencies of ∼5.5%. 10Despite the significant number of reports on DPP-based copolymers, there have been very few studies on the effect of modifying the 3,6-bis(5-bromothiophen-2-yl)-2,5-dialkylpyrrolo-[3,4-c]pyrrole-1,4-(2H,5H)-dione monomer. One very recent example was the replacement of the flanking thiophenes by furans, which resulted in polymers with high PCEs in solar cell devices. 11 We were interested in increasing the intermolecular association of DPP-based copolymers by repla...
High-performance, solution-processed transistors fabricated from semiconducting polymers containing indacenodithiohene repeat units are described. The bridging functions on the backbone contribute to suppressing large-scale crystallization in thin films. However, charge carrier mobilities of up to 1 cm(2)/(V s) for a benzothiadiazole copolymer were reported and, coupled with both ambient stability and long-wavelength absorption, make this family of polymers particularly attractive for application in next-generation organic optoelectronics.
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