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1 advances.sciencemag.org/cgi/content/full/2/1/e /dc1 Supplementary Materials for Efficient luminescent solar cells based on tailored mixed-cation perovskites Dongqin Bi, Wolfgang Tress, M. Ibrahim Dar, Peng Gao, Jingshan Luo, Clémentine Renevier, Kurt Schenk, Antonio Abate, Fabrizio Giordano, Juan-Pablo Correa Baena, Jean-David Decoppet, Shaik Mohammed Zakeeruddin, Mohammad Khaja Nazeeruddin, Michael Grätzel, Anders Hagfeldt The PDF file includes: Published 1 January 2016, Sci. Adv. 2, e (2016) DOI: /sciadv Fig. S1. Independent certification from Newport Corporation confirming PCEs of 19.90% (backward scan) and 19.73% (forward scan) and a normalized electroluminescence quantum efficiency. Fig. S2. Photograph of two real devices (front view and back view) showing the active area of the solar cell, the high reflectivity of the smooth gold electrode, and the densely opaque optical appearance of the perovskite film. Fig. S3. Histogram of solar cell efficiencies for 40 solar cells, with the optimized PbI2/FAI = Fig. S4. Initial stability test of PSCs sealed using epoxy and stored in a desiccator in the dark. Fig. S5. Absorption spectra of perovskite films on m-tio2/c-tio2/fto substrate with varying R measured in transmission. PbI 2 /FAI Fig. S6. Top-view SEM images of perovskite films on ms-tio2/c-tio2/fto with varying PbI2/FAI ratios (0.85, 1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solutions. Fig. S7. XRD patterns of perovskite films on ms-tio2/c-tio2/fto with varying PbI2/FAI ratios (0.85, 1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solutions. Fig. S8. Normalized (001) peaks of PbI2 phase showing the variation in full widths at half maximum with increasing ratios of PbI2/FAPbI3 fraction. Fig. S9. Cross-sectional SEM images of perovskite films on ms-tio2/c-tio2/fto with varying PbI2/FAI ratios (1, 1.05, 1.1, 1.23, 1.37, and 1.54) in the precursor solution.

2 Fig. S10. External electroluminescence quantum efficiency as a function of the injection current for the device with PbI2/FAI = Fig. S11. Normalized PL spectra of perovskite films on ms-tio2/bl-tio2/fto with varying PbI2/FAI ratios (1, 1.05, 1.1, 1.23, 1.37, and 1.54) in the precursor solution. Fig. S12. PL decay of perovskite films on ms-tio2/bl-tio2/fto with varying PbI2/FAI ratios (1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solution. Table S1. Photovoltaic parameters for PSCs measured using forward scan (from JSC to VOC) and backward scan (from VOC to JSC) at different scanning speeds (B, backward; F, forward). Table S2. Photovoltaic parameters for the stability of PSCs measured under AM 1.5 G illumination (solar cells were sealed with epoxy and stored in a dessicator). Table S3. Composition of perovskite composite film determined by Rietveld refinement.

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5 Fig. S1 Independent certification from Newport Corporation confirming PCEs of % (backward scan) and 19.73% (forward scan) and a normalized electroluminescence quantum efficiency. Fig. S2 Photograph of two real devices (front view and back view) showing the active area of the solar cell, the high reflectivity of the smooth gold electrode, and the densely opaque optical appearance of the perovskite film.

6 Fig. S3 Histogram of solar cell efficiencies for 40 solar cells, with the optimized PbI 2/FAI = Fig. S4 Initial stability test of PSCs sealed using epoxy and stored in a desiccator in the dark.

7 Table S1. Photovoltaic parameters for PSCs measured using forward scan (from JSC to VOC) and backward scan (from VOC to JSC) at different scanning speeds (B, backward; F, forward). Scanning speed Voc Jsc FF PCE (%) (mv/s) (ma/cm2) B F B F B F B F Table S2. Photovoltaic parameters for the stability of PSCs measured under AM 1.5 G illumination (solar cells were sealed with epoxy and stored in a dessicator). Voc Jsc (ma/cm2) FF PCE (%) initially After 216 h After 360 h After 648 h After 768 h

8 Fig. S5 Absorption spectra of perovskite films on m-tio 2/c-TiO 2/FTO substrate with varying R PbI 2 /FAI measured in transmission. This data was used to estimate the relative amount of perovskite by analyzing the absorbance spectra in the range between 550 and 700 nm after subtracting a background absorption due to the substrate. This wavelength range was chosen because PbI 2 and other FAPbI 3 phases do not show absorption in this range. The stoichiometric device, which showed the largest absorbance in that wavelength range, was used as reference. Dividing the other spectra by this spectrum gave a ratio independent of wavelength which corresponds in first approximation to the perovskite thickness if the absorption coefficient of the perovskite does not change.

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10 Fig. S6 Top-view SEM images of perovskite films on ms-tio 2/c-TiO 2/FTO with varying PbI 2/FAI ratios (0.85, 1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solutions.

11 Fig. S7 XRD patterns of perovskite films on ms-tio 2/c-TiO 2/FTO with varying PbI 2/FAI ratios (0.85, 1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solutions. Table S3. Composition of perovskite composite film determined by Rietveld refinement. Sample Film composition (Wt %) FWHM (001) Mean FWHM Mean Ratio of Ratio PbI2 Perovskite PbI2 [ ] Grain (011)/(101) Grain grain PbI2/FAI composites a Size FAPbI3 [ ] Size size [nm] [nm] (PbI2/FA I)

12 PbI a. It is very difficult to quantify the amount of bromide perovskite due to the formation of several different phases so we use perovskite composites to denote the rest of phases. Fig. S8 Normalized (001) peaks of PbI 2 phase showing the variation in full widths at half maximum with increasing ratios of PbI 2/FAPbI 3 fraction. Open circles and solid lines represent measured data and fit results, respectively.

13 Fig. S9 Cross-sectional SEM images of perovskite films on ms-tio 2/c-TiO 2/FTO with varying PbI 2/FAI ratios (1, 1.05, 1.1, 1.23, 1.37, and 1.54) in the precursor solution.

14 Fig. S10 External electroluminescence quantum efficiency as a function of the injection current for the device with PbI 2/FAI = The black line indicates a slope of 1.

15 Fig. S11 Normalized PL spectra of perovskite films on ms-tio 2/bl-TiO 2/FTO with varying PbI 2/FAI ratios (1, 1.05, 1.1, 1.23, 1.37, and 1.54) in the precursor solution. Excitation wavelength is 460 nm. The bandgap hardly shifts for samples with moderate PbI 2 excess.

16 Fig. S12 PL decay of perovskite films on ms-tio 2/bl-TiO 2/FTO with varying PbI 2/FAI ratios (1, 1.05, 1.1, 1.16, 1.23, 1.37, and 1.54) in the precursor solution. Pulsed source at 406 nm, and the samples were excited from perovskite side. The data shown in the main paper is corrected by subtracting the time-independent (in the time window below 2 µs) background signal.

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