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RISS 인기검색어
- 검색키워드
- 저자 : Calbo, Joaquí (검색결과 2 건)
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Intrinsic doping limit and defect-assisted luminescence in Cs4PbBr6
Jung, Young-Kwang,Calbo, Joaquí,n,Park, Ji-Sang,Whalley, Lucy D.,Kim, Sunghyun,Walsh, Aron The Royal Society of Chemistry 2019 Journal of Materials Chemistry A Vol.7 No.35
<P>Cs4PbBr6 is a member of the extended halide perovskite family that is built from isolated (zero-dimensional) PbBr6<SUP>4−</SUP> octahedra with Cs<SUP>+</SUP> counter ions. The material exhibits anomalous optoelectronic properties: optical absorption and weak emission in the deep ultraviolet (310-375 nm) with efficient luminescence in the green region (∼540 nm). Several hypotheses have been proposed to explain the giant Stokes shift including: (i) phase impurities; (ii) self-trapped exciton; (iii) defect emission. We explore, using first-principles theory and self-consistent Fermi level analysis, the unusual defect chemistry and physics of Cs4PbBr6. We find a heavily compensated system where the room-temperature carrier concentrations (<10<SUP>9</SUP> cm<SUP>−3</SUP>) are more than one million times lower than the defect concentrations. We show that the low-energy Br-on-Cs antisite results in the formation of a polybromide (Br3) species that can exist in a range of charge states. We further demonstrate from excited-state calculations that tribromide moieties are photoresponsive and can contribute to the observed green luminescence. Photoactivity of polyhalide molecules is expected to be present in other halide perovskite-related compounds where they can influence light absorption and emission.</P>
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Breathing-Dependent Redox Activity in a Tetrathiafulvalene-Based Metal–Organic Framework
Souto, Manuel,Romero, Jorge,Calbo, Joaquí,n,Vitó,rica-Yrezá,bal, Iñ,igo J.,Zafra, José,L.,Casado, Juan,Ortí,, Enrique,Walsh, Aron,Mí,nguez Espallargas, Guille American Chemical Society 2018 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.140 No.33
<P/><P>“Breathing” metal–organic frameworks (MOFs) that involve changes in their structural and physical properties upon an external stimulus are an interesting class of crystalline materials due to their range of potential applications including chemical sensors. The addition of redox activity opens up a new pathway for multifunctional “breathing” frameworks. Herein, we report the continuous breathing behavior of a tetrathiafulvalene (TTF)-based MOF, namely <B>MUV-2</B>, showing a reversible swelling (up to ca. 40% of the volume cell) upon solvent adsorption. Importantly, the planarity of the TTF linkers is influenced by the breathing behavior of the MOF, directly impacting on its electrochemical properties and thus opening the way for the development of new electrochemical sensors. Quantum chemical calculations and Raman spectroscopy have been used to provide insights into the tunability of the oxidation potential.</P>
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