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  • Layered Halide Double Perovskites: Dimensional Reduction of Cs2AgBiBr6 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Connor, B. A., Leppert, L., Smith, M. D., Neaton, J. B., Karunadasa, H. I. 2018; 140 (15): 5235–40


    We investigate the consequences of dimensional confinement on halide double perovskites by synthesizing two-dimensional analogues of the recently reported three-dimensional double perovskite Cs2AgBiBr6. The layered perovskites (BA)4AgBiBr8 (1) and (BA)2CsAgBiBr7 (2) (BA = CH3(CH2)3NH3+) feature metal-halide sheets of mono and bilayer thickness, respectively, where the ordered double-perovskite lattice is partitioned by organic cations. Electronic structure calculations indicate that the indirect bandgap of Cs2AgBiBr6 becomes direct when the infinitely thick inorganic lattice is reduced to monolayer thickness. Calculations on model systems allow us to separate the effects of dimensional reduction from those of the accompanying structural distortions in the inorganic sublattice. Detailed optical characterization shows that the photophysical properties of 1 and 2 are markedly different than those of their well-studied lead-halide analogs. Hybrid layered derivatives of double perovskites substantially expand on the substitutional flexibility of halide perovskites to encompass greater compositional and electronic diversity.

    View details for DOI 10.1021/jacs.8b01543

    View details for Web of Science ID 000430642000046

    View details for PubMedID 29575889

  • Charge Carrier Dynamics in Cs2AgBiBr6 Double Perovskite JOURNAL OF PHYSICAL CHEMISTRY C Bartesaghi, D., Slavney, A. H., Gelvez-Rueda, M. C., Connor, B. A., Grozema, F. C., Karunadasa, H. I., Savenije, T. J. 2018; 122 (9): 4809–16


    Double perovskites, comprising two different cations, are potential nontoxic alternatives to lead halide perovskites. Here, we characterized thin films and crystals of Cs2AgBiBr6 by time-resolved microwave conductance (TRMC), which probes formation and decay of mobile charges upon pulsed irradiation. Optical excitation of films results in the formation of charges with a yield times mobility product, φΣμ > 1 cm2/Vs. On excitation of millimeter-sized crystals, the TRMC signals show, apart from a fast decay, a long-lived tail. Interestingly, this tail is dominant when exciting close to the bandgap, implying the presence of mobile charges with microsecond lifetimes. From the temperature and intensity dependence of the TRMC signals, we deduce a shallow trap state density of around 1016/cm3 in the bulk of the crystal. Despite this high concentration, trap-assisted recombination of charges in the bulk appears to be slow, which is promising for photovoltaic applications.

    View details for DOI 10.1021/acs.jpcc.8b00572

    View details for Web of Science ID 000427331300008

    View details for PubMedID 29545908

    View details for PubMedCentralID PMC5846080