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- ItemCation exchange synthesis of AgBiS2 quantum dots for highly efficient solar cells(Cambridge : RSC Publ., 2024) Senina, Alina; Prudnikau, Anatol; Wrzesińska-Lashkova, Angelika; Vaynzof, Yana; Paulus, FabianSilver bismuth sulfide (AgBiS2) nanocrystals have emerged as a promising eco-friendly, low-cost solar cell absorber material. Their direct synthesis often relies on the hot-injection method, requiring the application of high temperatures and vacuum for prolonged times. Here, we demonstrate an alternative synthetic approach via a cation exchange reaction. In the first-step, bis(stearoyl)sulfide is used as an air-stable sulfur precursor for the synthesis of small, monodisperse Ag2S nanocrystals at room-temperature. In a second step, bismuth cations are incorporated into the nanocrystal lattice to form ternary AgBiS2 nanocrystals, without altering their size and shape. When implemented into photovoltaic devices, AgBiS2 nanocrystals obtained by cation exchange reach power conversion efficiencies of up to 7.35%, demonstrating the efficacy of the new synthetic approach for the formation of high-quality, ternary semiconducting nanocrystals.
- ItemSpectral dynamics of shift current in ferroelectric semiconductor SbSI(Washington : National Academy of Sciences, 2019) Sotome, M.; Nakamura, M.; Fujioka, J.; Ogino, M.; Kaneko, Y.; Morimoto, T.; Zhang, Y.; Kawasaki, M.; Nagaosa, N.; Tokura, Y.; Ogawa, N.Photoexcitation in solids brings about transitions of electrons/ holes between different electronic bands. If the solid lacks an inversion symmetry, these electronic transitions support spontaneous photocurrent due to the geometric phase of the constituting electronic bands: the Berry connection. This photocurrent, termed shift current, is expected to emerge on the timescale of primary photoexcitation process. We observe ultrafast evolution of the shift current in a prototypical ferroelectric semiconductor antimony sulfur iodide (SbSI) by detecting emitted terahertz electromagnetic waves. By sweeping the excitation photon energy across the bandgap, ultrafast electron dynamics as a source of terahertz emission abruptly changes its nature, reflecting a contribution of Berry connection on interband optical transition. The shift excitation carries a net charge flow and is followed by a swing over of the electron cloud on a subpicosecond timescale. Understanding these substantive characters of the shift current with the help of first-principles calculation will pave the way for its application to ultrafast sensors and solar cells.