SUPPLEMENTARY INFORMATION

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1 Filterless Narrowband Visible Photodetectors Qianqian Lin, Ardalan Armin, Paul L. Burn* and Paul Meredith* Centre for Organic Photonics & Electronics, School of Chemistry and Molecular Biosciences, and School of Mathematics and Physics, The University of Queensland, Brisbane, Queensland, Australia Requests for materials and all correspondences should be addressed to: NATURE PHOTONICS 1

2 Supporting figures Figure S1 Scanning Electron Microcopy (SEM) images of Rhodamine B-containing and neat organohalide perovskite films and photodiodes. (a) Rhodamine B- organohalide perovskite film top view. (b) Equivalent neat organohalide perovskite film top view. (c) and (e) Cross-sectional images of a Rhodamine B-organohalide perovskite narrowband photodiodes. (d) and (f) Cross-sectional images of the equivalent neat organohalide perovskite narrowband photodiodes. These images clearly show that the presence of the Rhodamine B hinders the formation of larger crystallites, decreasing the crystal size from 100~200 nm to <50 nm. Both the composite and neat organohalide perovskite films were uniform and continuous on ITO/PEDOT:PSS with thicknesses in the range 500~700 nm. 2 NATURE PHOTONICS

3 SUPPLEMENTARY INFORMATION Figure S2 X-ray Diffraction (XRD) and optical absorption of mixed organohalide perovskite CH 3NH 3PbI xbr 3-x thin films mixed with Rhodamine B. (a) XRD spectra of mixed organohalide perovskites. All of the spectra display the typical tetragonal perovskite crystal structure with (110) and (220) peaks around 14 and 29, respectively. (b) Comparison of XRD diffraction peaks corresponding to the (220) plane. The calculated interplanar spacing decreases with the increased content of PbBr 2 due to the smaller atomic radius of Br. (c) Absorption spectra of Rhodamine B doped mixed organohalide perovskites. The semiconductor band gap of the doped material can be tuned by mixing PbI 2 and PbBr 2 as per the neat material. The Rhodamine B concentration was fixed at 0.09 M and all organohalide perovskite precursor concentrations kept at 1 M. NATURE PHOTONICS 3

4 Figure S3 Static dielectric constant measurements of composite organohalide perovskite and mixed lead halide materials. (a) Red narrowband photodiode junction material (CH 3NH 3PbI 2Br) with r = 45. (b) Green narrowband photodiode junction material (CH 3NH 3PbIBr 2) with r = 35. (c) Blue narrowband photodiode junction material (PbI 1.4Br 0.6) with r = 19. All materials show high dielectric constants and large device capacitances indicating non-excitonic charge generation physics. 4 NATURE PHOTONICS

5 SUPPLEMENTARY INFORMATION k k n n Wavelength (nm) Figure S4 Optical constants (refractive index n and extinction coefficient k) of a Rhodamine B-CH 3NH 3PbI 2Br organohalide perovskite composite thin film. Precise optical constants were measured using spectroscopic ellipsometry and the values used for optical transfer matrix modeling. The extinction coefficient shows as expected two distinct regions, i.e., high and low k regimes. NATURE PHOTONICS 5

6 Figure S5 Noise analysis of an optimized red narrowband CCN photodiode (CH 3NH 3PbI 2Br-Rhodamine B). The plot shows the measured noise density as a function of reverse bias voltage obtained from the Fast Fourier Transform of the dark current as a function of time. For low reverse bias, the photodiode shows similar noise current ~100 fa Hz -1 as the high frequency range As prepared 2 months after encapsulation 4 months after encapsulation EQE (%) Wavelength (nm) Figure S6 Stability of an optimized red narrowband CCN photodiode (CH 3NH 3PbI 2Br- Rhodamine B). The devices were stored in air after encapsulation as described in the Methods section. The devices still work well as a red narrowband photodiodes despite having a higher response to blue and green light. 6 NATURE PHOTONICS

7 SUPPLEMENTARY INFORMATION Figure S7 XRD spectra of green and blue CCN narrowband photodiode junction active materials. Both PEIE-organohalide perovskite (CH 3NH 3PbIBr 2) and PEIE-lead halide (PbI 1.4Br 0.6) composite films show much lower XRD diffraction intensities and broader peaks, which confirm the decrease of crystal size. NATURE PHOTONICS 7

8 Figure S8 Device performance of RGB narrowband CCN photodiodes. (a), (b) and (c) show EQE spectra at different reverse bias voltages: red, blue and green photodiodes, respectively. The red photodiodes have relatively voltage independent behaviour, but the blue and green photodiodes have a more pronounced dependence. (d), (e) and (f) Display the temporal responses of the narrowband photodiodes to red, green and blue LED illumination, respectively. All of the photodiodes are high speed and show recovery within 10 s. 8 NATURE PHOTONICS

9 SUPPLEMENTARY INFORMATION Table S1 Typical dark currents (J d) and specific detectivities (D * ) of optimized RGB narrowband CCN photodiodes. J d at 0.2 V J d at 0.5 V D * at -0 V D * at -0.5 V (A/cm 2 ) (A/cm 2 ) (Jones) (Jones) Red photodiodes nm nm Green photodiodes nm nm Blue photodiodes nm nm NATURE PHOTONICS 9

10 Figure S9 Typical RC decay of a blue narrowband CCN photodiode. The current density decay was fitted by J = J 0+A*exp(-t/RC) to yield RC~0.4 s. All photodiodes exhibited similar RC decays (0.4~0.7 s) with R load = NATURE PHOTONICS

Electro-optics of perovskite solar cells

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