SUPPLEMENTARY INFORMATION - INFORMATION. DOI: 10.1038/NMAT4795. NATURE MATERIALS | . 1. 1 Graded band gap perovskite solar cells Supplementary

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    SUPPLEMENTARY INFORMATIONDOI: 10.1038/NMAT4795

    NATURE MATERIALS | www.nature.com/naturematerials 1

    1

    Graded band gap perovskite solar cells

    Supplementary Information

    Onur Ergen, 1,3,4 S.Matt Gilbert1, 3,4, ,Thang Pham1, 3,4 ,Sally J. Turner, 1,2,4, Mark Tian Zhi Tan 1, Marcus A. Worsley5 and Alex Zettl1, 3,4 1Department of Physics, University of California at Berkeley, Berkeley, California 94720, USA 2Department of Chemistry, University of California at Berkeley, Berkeley, California 94720, USA 3Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA 4Kavli Energy Nanosciences Institute at the University of California, Berkeley, and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA 5 Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA Corresponding Author: Prof. Alex Zettl (azettl@berkeley.edu) Supporting Information Content

    A) Material Characterization

    Absorption and Photoluminescence measurements SEM-EDAX study Top view SEM Images XRD patterns

    B) Electrical Characterization

    Current density vs. Time Hall Effect mobility measurements I-V curve of champion cell The reverse and forward sweep of perovskite cells Ohmic contact behavior of GaN NIR-PL spectra of graded band gap perovskite cells MASnI3 based solar cell with only GA modification EQE&IQE data of champion cell with integrated photocurrent Back surface pits on the GaN suface Mott-Schottky measurements GaN/Perovskite interface

    1

    Graded bandgap perovskite solar cells

    Supplementary Information

    Onur Ergen, 1,3,4 S.Matt Gilbert1, 3,4, ,Thang Pham1, 3,4 ,Sally J. Turner, 1,2,4, Mark Tian Zhi Tan 1, Marcus A. Worsley5 and Alex Zettl1, 3,4 1Department of Physics, University of California at Berkeley, Berkeley, California 94720, USA 2Department of Chemistry, University of California at Berkeley, Berkeley, California 94720, USA 3Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA 4Kavli Energy Nanosciences Institute at the University of California, Berkeley, and the Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA 5 Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA 94550, USA

    Corresponding Author:

    Prof. Alex Zettl (azettl@berkeley.edu)

    Supporting Information Content

    A) Material Characterization

    Absorption and Photoluminescence measurements SEM-EDAX study Top view SEM Images XRD patterns

    B) Electrical Characterization Current density vs. Time Hall Effect mobility measurements I-V curve of champion cell The reverse and forward sweep of perovskite cells Ohmic contact behavior of GaN NIR-PL spectra of graded band gap perovskite cells MASnI3 based solar cell with only GA modification EQE&IQE data of champion cell with integrated photocurrent Back surface pits on the GaN suface Mott-Schottky measurements GaN/Perovskite interface

    http://dx.doi.org/10.1038/nmat4795

  • 2016 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.

    2 NATURE MATERIALS | www.nature.com/naturematerials

    SUPPLEMENTARY INFORMATION DOI: 10.1038/NMAT4795

    2

    A) MaterialCharacterization

    Concentration variation

    Figure S 1 (a) UV-visible light absorption spectra of CH3NH3SnI3-xBrx and CH3NH3Pb(I1-xBrx)3, with varying iodide concentration x, b) Photoluminescence (PL), spectra of perovskite cells, CH3NH3SnI3-x and CH3NH3Pb(I1-xBrx)3, by varying iodide concentration x. The role of the graphene aerogels

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    x=1 x=0

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    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    2

    A) MaterialCharacterization

    Concentration variation

    Figure S 1 (a) UV-visible light absorption spectra of CH3NH3SnI3-xBrx and CH3NH3Pb(I1-xBrx)3, with varying iodide concentration x, b) Photoluminescence (PL), spectra of perovskite cells, CH3NH3SnI3-x and CH3NH3Pb(I1-xBrx)3, by varying iodide concentration x. The role of the graphene aerogels

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    Wavelength (nm)

    x=1 x=0

    x=1 x=0

    (a)

    (b)

    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    3

    (a) (b)

    (a) (b)

    (c) (d)

    Figure S 2 Photoluminescence analysis of perovskite cells in air (only CH3NH3PbI3-xBrx ). (a) without GA. (b) with GA modification. (c) Bandgap changing by time with and without GA layer. (d) EDAX line mapping for oxygen signature of a perovskite with and without GA modification. Graphene aerogel encapsulation acts as a barrier for oxygen penetration and moisture ingress.

    3

    (a) (b)

    (a) (b)

    (c) (d)

    Figure S 2 Photoluminescence analysis of perovskite cells in air (only CH3NH3PbI3-xBrx ). (a) without GA. (b) with GA modification. (c) Bandgap changing by time with and without GA layer. (d) EDAX line mapping for oxygen signature of a perovskite with and without GA modification. Graphene aerogel encapsulation acts as a barrier for oxygen penetration and moisture ingress.

    3

    (a) (b)

    (a) (b)

    (c) (d)

    Figure S 2 Photoluminescence analysis of perovskite cells in air (only CH3NH3PbI3-xBrx ). (a) without GA. (b) with GA modification. (c) Bandgap changing by time with and without GA layer. (d) EDAX line mapping for oxygen signature of a perovskite with and without GA modification. Graphene aerogel encapsulation acts as a barrier for oxygen penetration and moisture ingress.

    4

    The role of the h-BN

    Figure S 3(a) Top view SEM image of a perovskite sample after peeling off GA layer. The line formations arise due to interfacial adhesion. (b) Top view SEM image of samples without GA improvement. The scale bars in the SEM images are 5m.

    Figure S 4 XRD diffraction patterns of the perovskite layers of a) W/ GA and b) W/O GA.

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    10 25 40 60

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    2 (degree)

    2 (degree)

    (b)

    (a)

    W/ GA

    W/O GA

    http://dx.doi.org/10.1038/nmat4795

  • 2016 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.

    NATURE MATERIALS | www.nature.com/naturematerials 3

    SUPPLEMENTARY INFORMATIONDOI: 10.1038/NMAT4795

    2

    A) MaterialCharacterization

    Concentration variation

    Figure S 1 (a) UV-visible light absorption spectra of CH3NH3SnI3-xBrx and CH3NH3Pb(I1-xBrx)3, with varying iodide concentration x, b) Photoluminescence (PL), spectra of perovskite cells, CH3NH3SnI3-x and CH3NH3Pb(I1-xBrx)3, by varying iodide concentration x. The role of the graphene aerogels

    500 600 700 800 900 1000 1100

    Abs

    orba

    nce

    (a.u

    .)

    Wavelength (nm)

    1

    300 400 500 600 700 800 900 1000 1100 1200

    5

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    7

    Phot

    olum

    ines

    cenc

    e (a

    .u.)

    Wavelength (nm)

    x=1 x=0

    x=1 x=0

    (a)

    (b)

    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    CH3NH3Pb(I1-xBrx)3, x=0 CH3NH3Pb(I1-xBrx)3, x=0.045

    CH3NH3Pb(I1-xBrx)3, x=1

    CH3NH3Pb(I1-xBrx)3, x=0.5CH3NH3Pb(I1-xBrx)3, x=0.65

    CH3NH3Sn(I3-x)Brx, x=1CH3NH3Sn(I3-x)Brx, x=0

    2

    A) MaterialCharacterization

    Concentration variation

    Figure S 1 (a) UV-visible light absorption spectra of CH3NH3SnI3-xBrx and CH3NH3Pb(I1-xBrx)3, with varying iodide concentration x, b) Photoluminescence (PL), spectra of perovskite cells, CH3NH3SnI3-x and CH3NH

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