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    Optical Anisotropy and Momentum-Dependent Excitons in Dibenzopentacene Single Crystals
    (Washington, DC : ACS Publications, 2022) Graf, Lukas; Liu, Fupin; Naumann, Marco; Roth, Friedrich; Debnath, Bipasha; Büchner, Bernd; Krupskaya, Yulia; Popov, Alexey A.; Knupfer, Martin
    High-quality single crystals of the organic semiconductor (1,2;8,9)-dibenzopentacene were grown via physical vapor transport. The crystal structure─unknown before─was determined by single-crystal X-ray diffraction; polarization-dependent optical absorption measurements display a large anisotropy in the ac plane of the crystals. The overall Davydov splitting is ∼110 meV, which is slightly lower than that in the close relative pentacene (120 meV). Momentum-dependent electron energy-loss spectroscopy measurements show a clear exciton dispersion of the Davydov components. An analysis of the dispersion using a simple 1D model indicates smaller electron- and hole-transfer integrals in dibenzopentacene as compared to pentacene. The spectral weight distribution of the excitation spectra is strongly momentum-dependent and demonstrates a strong momentum-dependent admixture of Frenkel excitons, charge-transfer excitons, and vibrational modes.
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    A crystalline anionic complex of scandium nitride endometallofullerene: Experimental observation of single-bonded (Sc3N@Ih-C80−)2 dimers
    (Cambridge : Royal Society of Chemistry, 2016) Konarev, Dmitri V.; Zorina, Leokadiya V.; Khasanov, Salavat S.; Popov, Alexey A.; Otsuka, Akihiro; Yamochi, Hideki; Saito, Gunzi; Lyubovskaya, Rimma N.
    Reduction of scandium nitride clusterfullerene, Sc3N@Ih-C80, by sodium fluorenone ketyl in the presence of cryptand[2,2,2] allows the crystallization of the {cryptand[2,2,2](Na+)}2(Sc3N@Ih-C80−)2·2.5C6H4Cl2 (1) salt. The Sc3N@Ih-C80˙− radical anions are dimerized to form single-bonded (Sc3N@Ih-C80−)2 dimers.
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    A thiazolo[5,4-: D] thiazole-bridged porphyrin organic framework as a promising nonlinear optical material
    (London : Royal Society of Chemistry (RSC), 2019) Samal, Mahalaxmi; Valligatla, Sreeramulu; Saad, Nabil A.; Rao, M. Veeramohan; Rao, D. Narayana; Sahu, Rojalin; Biswal, Bishnu P.
    Porphyrin-based porous organic frameworks are an important group of materials gaining interest due to their structural diversity and distinct opto-electronic properties. However, these materials are seldom explored for nonlinear optical (NLO) applications. In this work, we investigate a thiazolo[5,4-d]thiazole-bridged porous, porphyrin framework (Por-TzTz-POF) with promising NLO properties. The planar TzTz moiety coupled with integrated porphyrin units enables efficient π-conjugation and charge distribution in the Por-TzTz-POF resulting in a high nonlinear absorption coefficient (β = 1100 cm GW-1) with figure of merit (FoM) σ1/σ0 = 5571, in contrast to analogous molecules and material counterparts e.g. metal-organic frameworks (MOFs; β = ∼0.3-0.5 cm GW-1), molecular porphyrins (β = ∼100-400 cm GW-1), graphene (β = 900 cm GW-1), and covalent organic frameworks (Por-COF-HH; β = 1040 cm GW-1 and FoM = 3534). This journal is © The Royal Society of Chemistry.
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    Perovskite phase heterojunction solar cells
    (London : Nature Publishing Group, 2022) Ji, Ran; Zhang, Zongbao; Hofstetter, Yvonne J.; Buschbeck, Robin; Hänisch, Christian; Paulus, Fabian; Vaynzof, Yana
    Modern photovoltaic devices are often based on a heterojunction structure where two components with different optoelectronic properties are interfaced. The properties of each side of the junction can be tuned by either utilizing different materials (for example, donor/acceptor) or doping (for example, p–n junction) or even varying their dimensionality (for example, 3D/2D). Here we demonstrate the concept of phase heterojunction (PHJ) solar cells by utilizing two polymorphs of the same material. We demonstrate the approach by forming γ-CsPbI3/β-CsPbI3 perovskite PHJ solar cells. We find that all of the photovoltaic parameters of the PHJ device significantly surpass those of each of the single-phase devices, resulting in a maximum power conversion efficiency of 20.1%. These improvements originate from the efficient passivation of the β-CsPbI3 by the larger bandgap γ-CsPbI3, the increase in the built-in potential of the PHJ devices enabled by the energetic alignment between the two phases and the enhanced absorption of light by the PHJ structure. The approach demonstrated here offers new possibilities for the development of photovoltaic devices based on polymorphic materials.