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SI-1 Supplementary Information (SI) Large area efficient interface layer free monolithic perovskite/homo-junction- silicon tandem solar cell with over 20% efficiency Jianghui Zheng 1, †,* , Cho Fai Jonathan Lau 1,† , Hamid Mehrvarz 1,† , Fa-Jun Ma 1 , Yajie Jiang 1 , Xiaofan Deng 1 , Anastasia Soeriyadi 1 , Jincheol Kim 1 , Meng Zhang 1 , Long Hu 1 , Xin Cui 1 , Da Seul Lee 1 , Jueming Bing 1 , Yongyoon Cho 1 , Chao Chen 2 , Martin A. Green 1 , Shujuan Huang 1 and Anita W. Y. Ho-Baillie 1,* 1 Australian Centre for Advanced Photovoltaics, School of Photovoltaic and Renewable Energy Engineering, University of New South Wales (UNSW), Sydney 2052, Australia 2 College of Energy, Xiamen University, Xiamen, 361005, China † These authors contribute equally to this work * Corresponding Author: Email: [email protected] (A. Ho-Baillie), [email protected] (J. Zheng) Electronic Supplementary Material (ESI) for Energy & Environmental Science. This journal is © The Royal Society of Chemistry 2018

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Page 1: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

SI-1

Supplementary Information (SI)Large area efficient interface layer free monolithic perovskite/homo-junction-silicon tandem solar cell with over 20% efficiency

Jianghui Zheng1, †,*, Cho Fai Jonathan Lau1,†, Hamid Mehrvarz1,†, Fa-Jun Ma1, Yajie Jiang1, Xiaofan Deng1, Anastasia Soeriyadi1, Jincheol Kim1, Meng Zhang1, Long Hu1, Xin Cui1, Da Seul Lee1, Jueming Bing1, Yongyoon Cho1, Chao Chen2, Martin A. Green1, Shujuan Huang1 and Anita W. Y. Ho-Baillie1,*

1 Australian Centre for Advanced Photovoltaics, School of Photovoltaic and Renewable Energy Engineering, University of New South Wales (UNSW), Sydney 2052, Australia2 College of Energy, Xiamen University, Xiamen, 361005, China

†These authors contribute equally to this work* Corresponding Author: Email: [email protected] (A. Ho-Baillie), [email protected] (J. Zheng)

Electronic Supplementary Material (ESI) for Energy & Environmental Science.This journal is © The Royal Society of Chemistry 2018

Page 2: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S1 (a) PCE, (b) FF, (c)JSC, (d)VOC, (e)Rs distributions for 12 opaque Au/ /spiro-OMeTAD/MAPbI3/SnO2/ITO glass PSC with different SnO2 thickness. The highest

value is a maximum value. The highest bar is the 75th percentile value. The middle bar is the median value. The square mark is for average. The lowest bar is the 25th

percentile value. The lowest value is the minimum. (f) J-V curve of the champion PSC device (with 0.159 cm2 active area) based on 15 nm SnO2 ETL.

Page 3: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method.

Fig. S3 XRD pattern of CH3NH3PbI3 layer deposited by 2 step method on glass.

Page 4: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S4 Cross sectional SEM images of the tandem devices with different thicknesses of CH3NH3PbI3 perovskite layer at (a) 260 nm; (b) 380 nm; (c) 470 nm.

Fig. S5 Simulated the EQE response of bottom silicon cell by changing the MAPbI3 thickness. Note that the SunSolveTM ray tracing package does not allow for carrier recombination input and therefore 100% IQE is assumed for both top perovskite and

bottom silicon solar cells which is not the case for experimental cells.

Page 5: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S6. XPS Si 2p spectrum of silicon surface after UVO treatment. The peak at 103.3 eV is attributed to SiO2 formed after UVO treatment, while the peak at 99.3 eV is

detected from the Si substrate underneath the thin oxide surface [10].

Page 6: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S7 Band diagrams of SnO2 and Si interface at the bias voltage of 0.4 V with different p++ doping concentration.

Fig. S8 AR foil fabrication process using rose petal. The thickness of the PDMS AR foil is around 2 mm.

Page 7: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S9 Reverse scan J-V curve of the 4 cm2 tandem device using heavier p++ front emitter for the Si bottom cell before (black) and after (red) the use of antireflection foil

on the front of the tandem.

Page 8: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

SI-8

Fig. S10 Simulated (solid line) and experimental (dotted line) EQE and 1-R for the demonstrated perovskite/silicon tandem. Note that the SunSolveTM ray tracing package does not allow for carrier recombination input and therefore 100% IQE is assumed for

both top perovskite and bottom silicon solar cells although it is not the case for experimental cells.

Page 9: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S11 Optical losses from each layer in the monolithic perovskite/silicon tandem.

Fig. S12 Measured transmittance of planar thin (0.3 mm) and thick (2.0 mm) PDMS layer showing the optical improvement from the use of thinner PDMS layer.

Page 10: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Fig. S13 Simulated EQE and total absorbance (1-reflectance; green line) of improved monolithic cell structure AR foil/Ag grid/ITO/NiOx/MAPbI3/SnO2/Silicon/SiO2/Ag.

Table S2: Breakdown of optical losses for the improved cell structure AR foil/Ag

grid/ITO/NiOx/MAPbI3/SnO2/Silicon/SiO2/Ag

Cell Layers Thickness JA (mA/cm2)

PDMS foil 0.3 mm 0.6

Front Ag grid 220 nm 0.2

ITO 100 nm 1.3

NiOx 20 nm 0.2

CH3NH3PbI3 381 nm 19.7

Perovskite top cell

SnO2 15 nm 0

Silicon 300 μm 19.7

SiO2 160 nm 0

Silicon bottom

Rear Ag 2 μm 0.2

Page 11: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

SI-11

Fig. S14 Simulated dark I-V curves for the SnO2/p++silicon interface without the presence of a native SiO2 when p++ doping concentration is varied. Inset: corresponding band diagram.

Page 12: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

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Table S1 Summaries of monolithic 2-terminal perovskite/silicon tandem device.

* certified by NREL;

Perovskite Eg (eV)

Silicon Interface layer

Voc(V)

Jsc(mA/c

m2)

FF PCE(%)

Stabilized PCE

(%)

Area(cm2)

Institute Publish month and

RefMAPbI3 1.55 Homojunction n++ Si

tunnel1.58 11.5 0.75 - 13.7 1.00 MIT/Sta

nford2015.03 [1]

MAPbI3 1.55 Homojunction ZTO 1.64 15.3 0.65 16.3 16.0 1.43 EPFL 2016.12 [2]CsRbFAMAPbI3-xBrx 1.62 Homojunction ITO 1.75 17.6 0.74 22.8 22.5 1.00 ANU 2017.10 [3]MAPbI3 1.58 Homojunction - 1.68 16.1 0.78 21.0 20.5 4.00MAPbI3 1.58 Homojunction - 1.66 15.6 0.68 17.6 17.1 16.00 UNSW This work

FAMAPbI3-xBrx 1.56 HIT ITO 1.79 14.0 0.77 19.1 18.1 0.16 HZB/EPFL

2015.10 [4]

MAPbI3 1.55 HIT IZO 1.69 15.9 0.78 20.9 21.2 0.17

MAPbI3 1.55 HIT IZO 1.70 16.1 0.71 19.5 19.2 1.22 EPFL 2015.12 [5]

MAPbI3 1.55 HIT IZO 1.72 16.4 0.73 20.6 20.5 1.43 EPFL 2016.07 [6]CsFAPbI3-xBrx 1.63 HIT ITO 1.65 18.1 0.79 23.6 23.6* 1.00 Stanford 2017.02 [7]CsFAPbI3-xBrx 1.63 HIT nc-Si

tunnel1.75 16.8 0.76 22.8 22.0 0.25

CsFAPbI3-xBrx 1.63 HIT nc-Si tunnel

1.78 16.5 0.74 21.8 21.2 1.43

CsFAPbI3-xBrx 1.63 HIT nc-Si tunnel

1.77 16.5 0.65 19.1 18.0 12.96

EPFL 2017.08 [8]

FAMAI3-xBrx 1.69 HIT ITO 1.73 15.3 0.79 20.6 18.0 0.03 PKU 2017.10 [9]

Page 13: Supplementary Information (SI) - rsc.org · SI-3 Fig. S2 Tauc plot and PL emission spectrum of CH3NH3PbI3 perovskite layer deposited by 2-step method. Fig. S3 XRD pattern of CH3NH3PbI3

SI-13

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[10] J. F. Moulder, W. F. Stickle, P. E. Sobol, and K. D. Bomben, Handbook of X-ray Photoelectron Spectroscopy, Perkin-Elmer Corp, USA (1992).


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