Volume 2, Issue 1, Pages 168-183 (January 2018) Highly Efficient and Stable Perovskite Solar Cells Enabled by All-Crosslinked Charge- Transporting Layers  Zonglong Zhu, Dongbing Zhao, Chu-Chen Chueh, Xueliang Shi, Zhongan Li, Alex K.-Y. Jen  Joule  Volume 2, Issue 1, Pages 168-183 (January 2018) DOI: 10.1016/j.joule.2017.11.006 Copyright © 2017 The Authors Terms and Conditions

Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions

Figure 1 Materials Synthesis and Characterization (A) The synthetic route of crosslinked c-HATNA via the thiol-ene thermal polymerization. (B) The first DSC scans of a blend of c-HATNA with and without PETMP by a heating rate of 10°C/min. (C) UV-visible spectra of the thin films before (black line) and after crosslinking (red line) at 110° ± 5°C for 30 min and solvent rinsing (blue line). (D–F) Energy-level diagram of complete PVSC layers with a typical planar p-i-n configuration of ITO/NiO/MAPbI3/c-HATNA/bis-C60/Ag (D); water contact angles of films of c-HATNA (E) and PCBM (F). (G) Photograph of the devices with PCBM (left) and c-HATNA (right) ETLs after exposure water droplet for 5 min. (H) Photograph of the devices with PCBM (left) and c-HATNA (right) ETLs after immersing in water for 5 min. Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions

Figure 2 Device Performance (A) Cross-sectional scanning electron microscopy image of complete PVSC layers with a typical planar p-i-n configuration of ITO/NiO/MAPbI3/c-HATNA/bis-C60/Ag. (B) J-V curves of perovskite solar cell with different ETLs. (C–E) SCLC mobility of different ETLs (C). Typical (D) J-V curves and (E) EQE of c-HATNA with 3 wt.% dopant with forward and reverse scanning direction. (F) The stabilized photocurrent density (black) and PCE (blue) obtained while holding the solar cell near the maximum power point voltage 0.91 V. (G) Histogram of efficiency distributions among 35 individual cells. Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions

Figure 3 Thermal and Illumination Stability (A–D) Thermal stability. Stability test of the PVSCs using crosslinked C- HATNA + 3 wt.% dopant (red) and PCBM as ETL (black) as a function of storage time under 70°C in nitrogen glovebox. All J-V curve measurements were tested in the nitrogen glovebox. (A) PCE, (B) VOC, (C) JSC, and (D) FF. (E–H) Illumination stability. The stability test of the PVSCs using crosslinked c-HATNA + 3 wt.% dopant (red) and PCBM as ETL (black) as a function of illumination time (AM 1.5 G illumination) at 70°C in ambient environment (air, humidity 50%–60%). (E) PCE, (F) VOC, (G) JSC, and (H) FF. Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions

Figure 4 All-Crosslinked CTLs-Based PVSCs on Rigid and Flexible ITO (A–G) Scheme (A) and energy diagram (B) of all-crosslinked PVSCs with ITO/c-TCTA/MAPbI3/c-HATNA/bis-C60/Ag; (C) the best J-V curve; and (D) the stabilized photocurrent density (black) and PCE (blue) of the all-crosslinked PVSCs obtained while holding the solar cell near the maximum power point voltage 0.84 V. Photograph (E), typical J-V curves (F), and stabilized photocurrent density (black) and PCE (red) (near the maximum power point voltage 0.79 V) (G) of all-crosslinked PVSCs. Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions

Figure 5 Stability Test of the PVSCs Using All-Crosslinked c-HATNA + 3wt.% Dopant (Red) and PCBM as ETL (Black) as a Function of Storage Time in Ambient Environment with 70°C Thermal Heating (A–D) All J-V curve measurements were tested in the nitrogen glovebox. (A) PCE, (B) VOC, (C) JSC, and (D) FF. Joule 2018 2, 168-183DOI: (10.1016/j.joule.2017.11.006) Copyright © 2017 The Authors Terms and Conditions