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Abstract:

The organic-inorganic hybrid perovskites methylammonium lead iodide (CH3NH3PbI3) and the partially chlorine-substituted mixed halide CH3NH3PbI3-xClx emit strong and broad photoluminescence (PL) around their band gap energy of ∼1.6 eV. However, the nature of the radiative decay channels behind the observed emission and, in particular, the spectral broadening mechanisms are still unclear. Here we investigate these processes for high-quality vapor-deposited films of CH3NH3PbI3-xClx using time- and excitation-energy dependent photoluminescence spectroscopy. We show that the PL spectrum is homogenously broadened with a line width of 103 meV most likely as a consequence of phonon coupling effects. Further analysis reveals that defects or trap states play a minor role in radiative decay channels. In terms of possible lasing applications, the emission spectrum of the perovskite is sufficiently broad to have potential for amplification of light pulses below 100 fs pulse duration.

Abstract:

The ability to process amorphous or polycrystalline solar cells at low temperature (<150 °C) opens many possibilities for substrate choice and monolithic multijunction solar cell fabrication. Organometal trihalide perovskite solar cells have evolved rapidly over the last two years, and the CH3NH3PbX3 (X = Cl, I or Br) material is processed at low temperature. However the first embodiments of the solar cell were composed of high temperature processed (500 °C) compact and mesoporous layers of TiO2. The sintering of the mesoporous TiO2 has been negated by replacing this with a mesoporous insulating scaffold in the meso-superstructured solar cell (MSSC), yet the high temperature processed compact TiO2 layer still persists in the most efficient devices. Here we have realised a low temperature route for compact TiO2, tailored for perovskite MSSC operation. With our optimized formulation we demonstrate full sun solar power conversion efficiencies of up to 15.9% in an all low temperature processed solar cell. © 2014 The Royal Society of Chemistry.

Abstract:

The ability to process amorphous or polycrystalline solar cells at low temperature (<150 °C) opens many possibilities for substrate choice and monolithic multijunction solar cell fabrication. Organometal trihalide perovskite solar cells have evolved rapidly over the last two years, and the CHNHPbX (X = Cl, I or Br) material is processed at low temperature. However the first embodiments of the solar cell were composed of high temperature processed (500 °C) compact and mesoporous layers of TiO. The sintering of the mesoporous TiO has been negated by replacing this with a mesoporous insulating scaffold in the meso-superstructured solar cell (MSSC), yet the high temperature processed compact TiO layer still persists in the most efficient devices. Here we have realised a low temperature route for compact TiO, tailored for perovskite MSSC operation. With our optimized formulation we demonstrate full sun solar power conversion efficiencies of up to 15.9% in an all low temperature processed solar cell. © The Royal Society of Chemistry 2014.

Abstract:

The highest efficiencies in solution-processable perovskite-based solar cells have been achieved using an electron collection layer that requires sintering at 500 °C. This is unfavorable for low-cost production, applications on plastic substrates, and multijunction device architectures. Here we report a low-cost, solution-based deposition procedure utilizing nanocomposites of graphene and TiO2 nanoparticles as the electron collection layers in meso-superstructured perovskite solar cells. The graphene nanoflakes provide superior charge-collection in the nanocomposites, enabling the entire device to be fabricated at temperatures no higher than 150 °C. These solar cells show remarkable photovoltaic performance with a power conversion efficiency up to 15.6%. This work demonstrates that graphene/metal oxide nanocomposites have the potential to contribute significantly toward the development of low-cost solar cells.

Abstract:

Solid-state dye-sensitized solar cells rely on effective infiltration of a solid-state hole-transporting material into the pores of a nanoporous TiO 2 network to allow for dye regeneration and hole extraction. Using microsecond transient absorption spectroscopy and femtosecond photoluminescence upconversion spectroscopy, the hole-transfer yield from the dye to the hole-transporting material 2,2′,7,7′-tetrakis(N,N-di-p- methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD) is shown to rise rapidly with higher pore-filling fractions as the dye-coated pore surface is increasingly covered with hole-transporting material. Once a pore-filling fraction of ≈30% is reached, further increases do not significantly change the hole-transfer yield. Using simple models of infiltration of spiro-OMeTAD into the TiO2 porous network, it is shown that this pore-filling fraction is less than the amount required to cover the dye surface with at least a single layer of hole-transporting material, suggesting that charge diffusion through the dye monolayer network precedes transfer to the hole-transporting material. Comparison of these results with device parameters shows that improvements of the power-conversion efficiency beyond ≈30% pore filling are not caused by a higher hole-transfer yield, but by a higher charge-collection efficiency, which is found to occur in steps. The observed sharp onsets in photocurrent and power-conversion efficiencies with increasing pore-filling fraction correlate well with percolation theory, predicting the points of cohesive pathway formation in successive spiro-OMeTAD layers adhered to the pore walls. From percolation theory it is predicted that, for standard mesoporous TiO2 with 20 nm pore size, the photocurrent should show no further improvement beyond an ≈83% pore-filling fraction. Solid-state dye-sensitized solar cells capable of complete hole transfer with pore-filling fractions as low as ∼30% are demonstrated. Improvements of device efficiencies beyond ∼30% are explained by a stepwise increase in charge-collection efficiency in agreement with percolation theory. Furthermore, it is predicted that, for a 20 nm pore size, the photocurrent reaches a maximum at ∼83% pore-filling fraction. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.