Preparation of Single-Phase Films of CH3NH3Pb(I1-xBrx)3 with Sharp Optical Band Edges.

Organometallic lead-halide perovskite-based solar cells now approach 18% efficiency. Introducing a mixture of bromide and iodide in the halide composition allows tuning of the optical bandgap. We prepare mixed bromide-iodide lead perovskite films CH3NH3Pb(I1-xBrx)3 (0 ≤ x ≤ 1) by spin-coating from solution and obtain films with monotonically varying bandgaps across the full composition range. Photothermal deflection spectroscopy, photoluminescence, and X-ray diffraction show that following suitable fabrication protocols these mixed lead-halide perovskite films form a single phase. The optical absorption edge of the pure triiodide and tribromide perovskites is sharp with Urbach energies of 15 and 23 meV, respectively, and reaches a maximum of 90 meV for CH3NH3PbI1.2Br1.8. We demonstrate a bromide-iodide lead perovskite film (CH3NH3PbI1.2Br1.8) with an optical bandgap of 1.94 eV, which is optimal for tandem cells of these materials with crystalline silicon devices.We acknowledge funding from the Engineering and Physical Sciences Research Council (EPSRC) and the Winton Programme (Cambridge) for the Physics of Sustainability. THT acknowledges funding from Cambridge Australia Scholarships and the Cambridge Commonwealth Trust. D.C. acknowledges support from St. John's College Cambridge and the Winton Programme (Cambridge) for the Physics of Sustainability.This is the final published version. It's also available at: http://pubs.acs.org/doi/abs/10.1021/jz501332v

Highly efficient and stable inverted perovskite solar cell employing PEDOT:GO composite layer as a hole transport layer

The beneficial use of a hole transport layer (HTL) as a substitution for poly(3,4-ethlyenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) is regarded as one of the most important approaches for improving the stability and efficiency of inverted perovskite solar cells. Here, we demonstrate highly efficient and stable inverted perovskite solar cells by applying a GO-doped PEDOT:PSS (PEDOT:GO) film as an HTL. The high performance of this solar cell stems from the excellent optical and electrical properties of the PEDOT:GO film, including a higher electrical conductivity, a higher work function related to the reduced contact barrier between the perovskite layer and the PEDOT:GO layer, enhanced crystallinity of the perovskite crystal, and suppressed leakage current. Moreover, the device with the PEDOT:GO layer showed excellent long-term stability in ambient air conditions. Thus, the enhancement in the efficiency and the excellent stability of inverted perovskite solar cells are promising for the eventual commercialization of perovskite optoelectronic devices

Impact of Molecular Charge-Transfer States on Photocurrent Generation in Solid State Dye-Sensitized Solar Cells Employing Low-Band-Gap Dyes

"Push-pull" structures have been considered a winning strategy for the design of fully organic molecules as sensitizers in dye-sensitized solar cells (DSSC). In this work we show that the presence of a molecular excited state with a strong charge-transfer character may be critical for charge generation when the total energy of the photoexcitation is too low to intercept accepting states in the TiO2 photoanode. Though hole transfer to the 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9, 9′-spirobifluorene can be very fast, an electron-hole pair is likely to form at the organic interface, resulting in a possible traplike excitation. This leads to poor photocurrent generation in the solid state DSSC (ss-DSSC) device. We demonstrate that it is possible to overcome this issue by fabricating SnO2-based ss-DSSC. The resulting solar cell shows, for the first time, that a SnO2-based ss-DSSC can outperform a TiO 2-based one when a perylene-based, low-band-gap, push-pull dye is used as sensitizer. © 2014 American Chemical Society

Lead-free organic–inorganic tin halide perovskites for photovoltaic applications

Already exhibiting solar to electrical power conversion efficiencies of over 17%, organic-inorganic lead halide perovskite solar cells are one of the most promising emerging contenders in the drive to provide a cheap and clean source of energy. One concern however, is the potential toxicology issue of lead, a key component in the archetypical material. The most likely substitute is tin, which like lead, is also a group 14 metal. While organic-inorganic tin halide perovskites have shown good semiconducting behaviour, the instability of tin in its 2+ oxidation state has thus far proved to be an overwhelming challenge. Here, we report the first completely lead-free, CH3NH 3SnI3 perovskite solar cell processed on a mesoporous TiO2 scaffold, reaching efficiencies of over 6% under 1 sun illumination. Remarkably, we achieve open circuit voltages over 0.88 V from a material which has a 1.23 eV band gap

Lead-free organic-inorganic tin halide perovskites for photovoltaic applications

Already exhibiting solar to electrical power conversion efficiencies of over 17%, organic-inorganic lead halide perovskite solar cells are one of the most promising emerging contenders in the drive to provide a cheap and clean source of energy. One concern however, is the potential toxicology issue of lead, a key component in the archetypical material. The most likely substitute is tin, which like lead, is also a group 14 metal. While organic-inorganic tin halide perovskites have shown good semiconducting behaviour, the instability of tin in its 2+ oxidation state has thus far proved to be an overwhelming challenge. Here, we report the first completely lead-free, CH3NH 3SnI3 perovskite solar cell processed on a mesoporous TiO2 scaffold, reaching efficiencies of over 6% under 1 sun illumination. Remarkably, we achieve open circuit voltages over 0.88 V from a material which has a 1.23 eV band gap. This journal is © the Partner Organisations 2014

Lead-free organic–inorganic tin halide perovskites for photovoltaic applications

Already exhibiting solar to electrical power conversion efficiencies of over 17%, organic-inorganic lead halide perovskite solar cells are one of the most promising emerging contenders in the drive to provide a cheap and clean source of energy. One concern however, is the potential toxicology issue of lead, a key component in the archetypical material. The most likely substitute is tin, which like lead, is also a group 14 metal. While organic-inorganic tin halide perovskites have shown good semiconducting behaviour, the instability of tin in its 2+ oxidation state has thus far proved to be an overwhelming challenge. Here, we report the first completely lead-free, CH3NH 3SnI3 perovskite solar cell processed on a mesoporous TiO2 scaffold, reaching efficiencies of over 6% under 1 sun illumination. Remarkably, we achieve open circuit voltages over 0.88 V from a material which has a 1.23 eV band gap. This journal is © the Partner Organisations 2014

Electron–phonon coupling in hybrid lead halide perovskites

Phonon scattering limits charge-carrier mobilities and governs emission line broadening in hybrid metal halide perovskites. Establishing how charge carriers interact with phonons in these materials is therefore essential for the development of high-efficiency perovskite photovoltaics and low-cost lasers. Here we investigate the temperature dependence of emission line broadening in the four commonly studied formamidinium and methylammonium perovskites, HC(NH2)2PbI3, HC(NH2)2PbBr3, CH3NH3PbI3 and CH3NH3PbBr3, and discover that scattering from longitudinal optical phonons via the Fröhlich interaction is the dominant source of electron-phonon coupling near room temperature, with scattering off acoustic phonons negligible. We determine energies for the interacting longitudinal optical phonon modes to be 11.5 and 15.3 meV, and Fröhlich coupling constants of ∼40 and 60 meV for the lead iodide and bromide perovskites, respectively. Our findings correlate well with first-principles calculations based on many-body perturbation theory, which underlines the suitability of an electronic band-structure picture for describing charge carriers in hybrid perovskites