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A new series of triphenylamine (TPA)‐functionalized isomeric polythiophenes are developed as hole transporting materials (HTM) for inverted tin‐based perovskite solar cells (TPSCs). Bithiophene (BT) is first functionalized with two TPA (electron donor; D) at 3 and 5 positions to give two structural isomeric compounds (3BT2D and 5BT2D). The functionalized BT2Ds are then coupled with 3,3′‐bis(tetradecylthio)‐2,2′‐bithiophene (SBT‐14)/3,3′‐ditetradecyl‐2,2′‐bithiophene (BT‐14) to produce structural isomeric polythiophenes (1‐4), which are compared to conventional poly[N,N″‐bis(4‐butylphenyl)‐N,N″‐bis(phenyl)‐benzidine] (poly‐TPD) as HTMs for TPSCs. With the appropriate alignment of energy levels with regard to the perovskite layer, the TPA‐functionalized polymers‐based TPSCs exhibit enhanced operational stability and efficiency. Moreover, the long thiotetradecyl chain in SBT‐14 with intramolecular S(alkyl)∙∙∙S(thio) interactions restricts the molecular rotation and has a strong impact on the molecular solubility and wettability of the film during device fabrication. Among all the polymers studied, TPSCs fabricated with 3‐SBT‐BT2D polymer exhibit the highest hole mobility as well as the slowest charge recombination and achieve the highest power conversion efficiency of 8.6%, with great long‐term stability for the performance retaining ≈90% of its initial values for shelf storage over 4000 h, which is the best efficiency for non‐PEDOT:PSS‐based TPSCs ever reported. [ABSTRACT FROM AUTHOR]

Three new donor-π-donor (D-π-D) tetrathienoacene (thieno[2′,3′:4,5]thieno[3,2- b]thieno[2,3- d]thiophene (TTA))-cored chromophores, end-functionalized with electron-donating triphenylamine (TPA) groups, were developed and characterized for their two-photon-related properties by using both nano- and femtosecond laser pulses as the probing tools. TTA-based chromophores exhibit stronger and more widely dispersed two-photon absorption (2PA) than those of dithienothiophene (DTT)-based congeners. As a consequence, the bithiophene-conjugated TTA chromophore exhibits the highest maximum 2PA cross-section value (up to 2500 GM) with good thermal stability, and thus, it is the best performing two-photon chromophore among the studied model compounds. The bithiophene-conjugated DTT analogue exhibits the second highest maximum two-photon absorptivity of 1950 GM, which is nearly 7 times larger than that of previously reported DTT-based chromophores. [ABSTRACT FROM AUTHOR]

Developing efficient interfacial hole transporting materials (HTMs) is crucial for achieving high‐performance Pb‐free Sn‐based halide perovskite solar cells (PSCs). Here, a new series of benzodithiophene (BDT)‐based organic small molecules containing tetra‐ and di‐triphenyl amine donors prepared via a straightforward and scalable synthetic route is reported. The thermal, optical, and electrochemical properties of two BDT‐based molecules are shown to be structurally and energetically suitable to serve as HTMs for Sn‐based PSCs. It is reported here that ethylenediammonium/formamidinium tin iodide solar cells using BDT‐based HTMs deliver a champion power conversion efficiency up to 7.59%, outperforming analogous reference solar cells using traditional and expensive HTMs. Thus, these BDT‐based molecules are promising candidates as HTMs for the fabrication of high‐performance Sn‐based PSCs. [ABSTRACT FROM AUTHOR]

Four new asymmetric donor-π-acceptor (D-π-A) fused-thiophene based chromophores were developed and characterized for a two-photon absorption study. In the chromophores the alkylated tetrathienoacene served as a π spacer, p -methoxytriphenylamine was used as an electron donor, and a cyanoalkyl acetate unit was employed as the acceptor. To investigate the effect of elongated conjugation on this system, thiophene units were systematically incorporated between the central core and each capped ends. The thermal, optical, and electrochemical properties of these compounds were investigated. The photo-physical, electrochemical and electronic properties of these molecules were compared, and all four chromophores exhibit strong fluorescence and high thermal stability. The elucidated structure-property correlations are in agreement with the theoretical calculations based on the density functional theory. The compound containing a thiophene unit between the donor and spacer exhibits a maximal two-photon absorption cross-section value of 1130 GM. [ABSTRACT FROM AUTHOR]