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  • 1.
    Adranno, Brando
    et al.
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden..
    Renier, Olivier
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden..
    Bousrez, Guillaume
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden.;Linköping Univ, Dept Sci & Technol, Lab Organ Elect, S-60174 Norrköping, Sweden..
    Paterlini, Veronica
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden..
    Baryshnikov, Glib V.
    Smetana, Volodymyr
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden..
    Tang, Shi
    Umeå Univ, Organ Photon & Elect Grp, S-90187 Umeå, Sweden..
    Ågren, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Chemical and Bio-Molecular Physics.
    Metlen, Andreas
    Queens Univ Belfast, QUILL Res Ctr, Sch Chem & Chem Engn, Belfast BT95AG, North Ireland..
    Edman, Ludvig
    Umeå Univ, Organ Photon & Elect Grp, S-90187 Umeå, Sweden..
    Anja-Verena, Mudring
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden.;Aarhus Univ, Dept Biol & Chem Engn & iNANO, Intelligent Adv Mat iAM, DK-8000 Aarhus, Denmark..
    Rogers, Robin D.
    Stockholm Univ, Dept Mat & Environm Chem, Svante Arrhenius vag 16C, S-10691 Stockholm, Sweden.;Queens Univ Belfast, QUILL Res Ctr, Sch Chem & Chem Engn, Belfast BT95AG, North Ireland.;Univ Alabama, Dept Chem & Biochem, Tuscaloosa, AL 35487 USA..
    The 8-Hydroxyquinolinium Cation as a Lead Structure for Efficient Color-Tunable Ionic Small Molecule Emitting Materials2023In: ADVANCED PHOTONICS RESEARCH, ISSN 2699-9293, Vol. 4, no 3, article id 2200279Article in journal (Refereed)
    Abstract [en]

    Albeit tris(8-hydroxyquinolinato) aluminum (Alq(3)) and its derivatives are prominent emitter materials for organic lighting devices, and the optical transitions occur among ligand-centered states, the use of metal-free 8-hydroxyquinoline is impractical as it suffers from strong nonradiative quenching, mainly through fast proton transfer. Herein, it is shown that the problem of rapid proton exchange and vibration quenching of light emission can be overcome not only by complexation, but also by organization of the 8-hydroxyquinolinium cations into a solid rigid network with appropriate counter-anions (here bis(trifluoromethanesulfonyl)imide). The resulting structure is stiffened by secondary bonding interactions such as pi-stacking and hydrogen bonds, which efficiently block rapid proton transfer quenching and reduce vibrational deactivation. Additionally, the optical properties are tuned through methyl substitution from deep blue (455 nm) to blue-green (488 nm). Time-dependent density functional theory (TDFT) calculations reveal the emission to occur from which an unexpectedly long-lived S-1 level, unusual for organic fluorophores. All compounds show comparable, even superior photoluminescence compared to Alq(3) and related materials, both as solids and thin films with quantum yields (QYs) up to 40-50%. In addition, all compounds show appreciable thermal stability with decomposition temperatures above 310 degrees C.

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  • 2.
    Grilli, Davide
    et al.
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;Univ Genoa, Dept Chem & Ind Chem, DCCI, I-16146 Genoa, Italy.;Inst SPIN CNR, I-16152 Genoa, Italy..
    Smetana, Volodymyr
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;Dept Biol & Chem Engn, DK-8000 Aarhus C, Denmark.;iNANO, DK-8000 Aarhus C, Denmark..
    Ahmed, Sheikh J.
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;Dept Biol & Chem Engn, DK-8000 Aarhus C, Denmark.;iNANO, DK-8000 Aarhus C, Denmark..
    Shtender, Vitalii
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry.
    Pani, Marcella
    Univ Genoa, Dept Chem & Ind Chem, DCCI, I-16146 Genoa, Italy.;Inst SPIN CNR, I-16152 Genoa, Italy..
    Manfrinetti, Pietro
    Univ Genoa, Dept Chem & Ind Chem, DCCI, I-16146 Genoa, Italy.;Inst SPIN CNR, I-16152 Genoa, Italy..
    Mudring, Anja-Verena
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;Dept Biol & Chem Engn, DK-8000 Aarhus C, Denmark.;iNANO, DK-8000 Aarhus C, Denmark..
    Lan(n+1)+xNin(n+5)+ySi(n+1)(n+2)–z: A Symmetric Mirror Homologous Series in the La-Ni-Si System2023In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 62, no 27, p. 10736-10742Article in journal (Refereed)
    Abstract [en]

    A homologous series La n(n+1)+x Ni n(n+5)+y Si(n+1)(n+2)-z has beenobserved inthe La-Ni-Si representing a symmetric Ni-rich mirrorto the La(n+1)(n+2)Ni n(n-1)+2Si n(n+1). A series of fourhomologous silicides have been discovered duringsystematic explorations in the central part of the La-Ni-Sisystem at 1000 & DEG;C. All compounds La12.5Ni28.0Si18.3 (n = 3; a = 28.8686(8), c = 4.0737(2) & ANGS;, Z = 3), La22.1Ni39.0Si27.8 (n = 4; a = 20.9340(6), c = 4.1245(2) & ANGS;, Z = 1), La32.9Ni49.8Si39.3 (n = 5; a = 24.946(1), c = 4.1471(5) & ANGS;, Z = 1), and La44.8Ni66.1Si53.4 (n =6; a = 28.995(5), c = 4.158(1) & ANGS;, Z = 1) crystallize in the hexagonal space group P6(3)/m and can be generalizedaccording to La n(n+1)+x Ni n(n+5)+y Si(n+1)(n+2)-z with n = 3-6. Their crystalstructures are based on AlB2-type building blocks, fusedLa-centered Ni6Si6 hexagonal prisms, yieldinglarger oligomeric equilateral domains with the edge size equal to n. The domains extend along the c axisand show checkered ordering of the cationic and anionic parts, whileall their atoms are located on mirror planes. La n(n+1)+x Ni n(n+5)+y Si(n+1)(n+2)-z can beconsidered as a mirror series to the La-rich La(n+1)(n+2)Ni n(n-1)+2Si n(n+1), where an exchange of the formal cationic and anionic sites,i.e., La and Si, occurs. The La-Ni-Si system is thefirst system where two such analogous series have been observed.

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  • 3.
    Pani, Marcella
    et al.
    Univ Genoa, Dept Chem & Ind Chem, DCCI, Via Dodecaneso 31, I-16146 Genoa, Italy.;CNR SPIN, Corso Perrone 24, I-16152 Genoa, Italy..
    Provino, Alessia
    Univ Genoa, Dept Chem & Ind Chem, DCCI, Via Dodecaneso 31, I-16146 Genoa, Italy.;CNR SPIN, Corso Perrone 24, I-16152 Genoa, Italy..
    Smetana, Volodymyr
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Shtender, Vitalii
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Bernini, Cristina
    CNR SPIN, Corso Perrone 24, I-16152 Genoa, Italy..
    Mudring, Anja-Verena
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;253 Aarhus Univ, Dept Chem, DK-8000 Aarhus C, Denmark.;253 Aarhus Univ, iNANO, DK-8000 Aarhus C, Denmark..
    Manfrinetti, Pietro
    Univ Genoa, Dept Chem & Ind Chem, DCCI, Via Dodecaneso 31, I-16146 Genoa, Italy.;CNR SPIN, Corso Perrone 24, I-16152 Genoa, Italy..
    Four ternary silicides in the La-Ni-Si system: from polyanionic layers to frameworks2022In: CrystEngComm, ISSN 1466-8033, E-ISSN 1466-8033, Vol. 24, no 47, p. 8219-8228Article in journal (Refereed)
    Abstract [en]

    The central part of the La-Ni-Si system has been investigated at 800 degrees C by means of single crystal X-ray diffraction, microscopy and analytical microprobe techniques. The result led to the identification of four new metal-rich silicides: LaNi2Si (R3m, a = 4.0263(3) angstrom, c = 15.066(2) angstrom, Z = 3), La2Ni3Si2 (P2(1)/c, a = 6.8789(7) angstrom, b = 6.2167(3) angstrom, c = 12.214(1) angstrom, beta = 90.92(1), Z = 4), La3Ni3Si2 (Pnma, a = 7.501(2) angstrom, b = 14.316(4) angstrom, c = 6.149(2) angstrom, Z = 4), La6Ni7Si4 (Pbcm, a = 6.066(1) angstrom, b = 7.488(1) angstrom, c = 29.682(5) angstrom, Z = 4). LaNi2Si belongs to the SrCu2Ga structure type, which is not represented among silicides, while La2Ni3Si2 crystallizes in its own structure type. Both compounds feature layered polyanionic motifs consisting of Ni and Si, which are separated by La. Instead, La6Ni7Si4 and La3Ni3Si2 are characterized by polyanionic networks. The former compound belongs to the Pr6Ni7Si4 structure type, with only two other representatives (Ce and Nd); the latter has been observed only with Rh and Ir. The two structures reveal close structural relationships having multiple identical slabs. Tight-binding electronic structure calculations by linear muffin-tin-orbital methods were performed for LaNi2Si, La2Ni3Si2 and La3Ni3Si2 to gain insights into their structure-bonding relationships. Their band structures suggest a metallic character for all compounds. The overall crystal orbital Hamilton populations are dominated by polar Ni-Si bonds, though homoatomic Ni-Ni and La-Ni(Si) bond contributions are not negligible. The variety of bonding patterns may serve as a logical explanation for the number of discovered compounds in this system as well as for the diversity of the observed structures.

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  • 4.
    Renier, Olivier
    et al.
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Bousrez, Guillaume
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Baryshnikov, Glib V.
    KTH Royal Inst Technol, Sch Engn Sci Chem, Div Theoret Chem & Biol, Biotechnol & Hlth, S-10691 Stockholm, Sweden.;Linköping Univ, Dept Sci & Technol, Lab Organ Elect, SE-60174 Norrköping, Sweden..
    Paterlini, Veronica
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Smetana, Volodymyr
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Ågren, Hans
    Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Chemical and Bio-Molecular Physics.
    Rogers, Robin D.
    Univ Alabama, Coll Arts & Sci, Tuscaloosa, AL 35487 USA..
    Mudring, Anja-Verena
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden.;Aarhus Univ, Dept Chem & iNANO, DK-8000 Aarhus, Denmark..
    Shape Preserving Single Crystal to Amorphous to Single Crystal Polymorphic Transformation Is Possible2021In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 143, no 48, p. 20202-20206Article in journal (Refereed)
    Abstract [en]

    Many crystalline materials form polymorphs and undergo solid-solid transitions between different forms as a function of temperature or pressure. However, there is still a poor understanding of the mechanism of transformation. Conclusions about the transformation process are typically drawn by comparing the crystal structures before and after the conversion, but gaining detailed mechanistic knowledge is strongly impeded by the generally fast rate of these transitions. When the crystal morphology does not change, it is assumed that crystallinity is maintained throughout the process. Here we report transformation between polymorphs of ZnCl2(1,3-diethylimidazole-2-thione)(2) which are sufficiently slow to allow unambiguous assignment of single crystal to single crystal transformation with shape preservation proceeding through an amorphous intermediate phase. This result fundamentally challenges the commonly accepted views of polymorphic phase transition mechanisms.

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  • 5.
    Shtender, Vitalii
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Smetana, Volodymyr
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Crivello, Jean-Claude
    Univ Paris Est Creteil, CNRS, ICMPE, F-94320 Thiais, France..
    Gondek, Lukasz
    AGH Univ Sci & Technol, Fac Phys & Appl Comp Sci, PL-30059 Krakow, Poland..
    Przewozznik, Janusz
    AGH Univ Sci & Technol, Fac Phys & Appl Comp Sci, PL-30059 Krakow, Poland..
    Mudring, Anja-Verena
    Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden..
    Sahlberg, Martin
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström.
    Honeycomb Constructs in the La-Ni Intermetallics: Controlling Dimensionality via p-Element Substitution2023In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 62, no 37, p. 14843-14851Article in journal (Refereed)
    Abstract [en]

    The new ternary compounds La15Ni13Bi5 and La9Ni8Sn5 were obtained by arc melting under argon from appropriate amounts of the elements and subsequent annealing at 800 degrees C for 2 weeks. Single-crystal X-ray diffraction reveals that they represent two new structure types: La15Ni13Bi5 crystallizes in the hexagonal space group P62m [hP33, a = 14.995(3), c = 4.3421(10) Å, V = 845.5(4) Å3, Z = 1] and La9Ni8Sn5 in P63/m [hP88, a = 23.870(15), c = 4.433(3) Å, V = 2187(3) Å3, Z = 4]. The crystal structures of both compounds are characterized by hexagonal honeycomb-based motifs formed by Ni and Sn that extend along the c axis. The building motif with its three-blade wind turbine shape is reminiscent of the organic molecule triptycene and is unprecedented in extended solids. First-principles calculations have been performed in order to analyze the electronic structure and provide insight into chemical bonding. They reveal significant electron transfer from La to Ni and the respective p-element, which supports the formation of the polyanionic Ni-p-element network. DFT calculations suggest paramagnetic-like behavior for both compounds, which was confirmed by magnetic measurements.

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