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Ultrahydrophobic 3D/2D fluoroarene bilayer-based water-resistant perovskite solar cells with efficiencies exceeding 22%

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Science Advances  07 Jun 2019:
Vol. 5, no. 6, eaaw2543
DOI: 10.1126/sciadv.aaw2543
  • Fig. 1 Experimental strategy and elemental and morphological analysis of 3D/2D perovskite bilayer.

    (A) Schematic illustration of the 2D treatment of 3D perovskite to form the 3D/2D bilayer perovskite with the structural representation of the FEA+ cation and the corresponding optimized geometry [density functional theory (DFT) calculation on B3LYP/6-31G(d) level of theory]. (B and C) Structures of pure 3D perovskite and pure 2D perovskite, respectively. (D) Fluorine XPS in-depth profiling of a 3D/2D bilayer perovskite. (E and F) SEM images of a pure 3D and an FEAI-treated 3D/2D perovskite film, respectively. Scale bars, 1000 nm.

  • Fig. 2 Structural and spectroscopic characterization of 3D/2D perovskite bilayer.

    Structural characterizations of perovskite films. (A) XRR data of pure 2D, 3D, and 3D/2D perovskite films. a.u., arbitrary unit. (B) GIXD data of pure 2D, 3D, and 3D/2D perovskite films. The angle of incidence is 0.14°, which is slightly above the critical angle at the used x-ray energy (22 keV). (C to E) GIWAXS data of 3D, 3D/2D, and pure 2D perovskite films (angle of incidence = 0.1°). Green and orange circles denote the 2D-β and 2D-γ structures, respectively. (F) Radially integrated intensity of GIWAXS data at two different angles of incidences to change between bulk (0.2°) and surface (0.1°) sensitivity. (G) TRPL decay traces recorded from the 3D and 3D/2D perovskite films.

  • Fig. 3 Device architecture, photovoltaic performance, and operational stability of 3D/2D bilayer PSCs.

    (A) Cross-sectional SEM of a 3D/2D PSC. (B) I-V curves of a 3D PSC and a 3D/2D PSC, with inset showing MPP tracking. (C) IPCE curves of a 3D PSC and a 3D/2D PSC. (D) Plot of contact resistance against voltage. (E) Ambient atmosphere aging results of a 3D PSC and a 3D/2D PSC, with the relative humidity shown in the inset. (F and G) Images of water droplets on the surface of 3D/2D and 3D perovskite films at different water loading times.

  • Table 1 Photovoltaic parameters of 3D/2D and 3D PSCs (measured under simulated AM 1.5G solar irradiance at 100 mW cm−2).

    PSCVOC (V)FF (%)JSC (mA cm−2)PCE (%)PCEMPP* (%)
    3D/2D1.096 (1.095)78.4 (76.9)25.79 (25.81)22.16 (21.70)22.09
    3D1.045 (1.036)77.5 (75.1)25.47(25.47)20.62 (19.74)19.97

    *MPP tracking. The efficiencies are recorded after 140-s MPP tracking.

    †The brackets indicate the average values of 25 PSC devices.

    Supplementary Materials

    • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/5/6/eaaw2543/DC1

      Fig. S1. UV-vis absorption spectrum of 3D and 3D/2D perovskite films and geometry of FEA+ cation.

      Fig. S2. Surface and in-depth elemental analyses of 3D/2D perovskite bilayer.

      Fig. S3. Cross-comparison of the GIWAXS patterns on surface and in bulk for 3D and 3D/2D perovskites, respectively.

      Fig. S4. Steady-state PL of 3D and 3D/2D perovskite systems.

      Fig. S5. Hole injection dynamics and band diagram of the 3D/2D perovskite system.

      Fig. S6. JSC, VOC, FF, and PCE distributions of 50 devices, in which 25 devices are 3D/2D PSCs and 25 are 3D PSCs.

      Fig. S7. Impedance spectroscopy and capacitance measurement of 3D and 3D/2D PSCs.

      Fig. S8. Water and humidity resistance of 3D/2D and 3D PSCs.

      Fig. S9. Image of water droplet on the surface of pure 2D [(FEAI)2PbI4] perovskite films.

      Fig. S10. Stability of a 3D/2D PSC and a 3D PSC at an elevated temperature.

    • Supplementary Materials

      This PDF file includes:

      • Fig. S1. UV-vis absorption spectrum of 3D and 3D/2D perovskite films and geometry of FEA+ cation.
      • Fig. S2. Surface and in-depth elemental analyses of 3D/2D perovskite bilayer.
      • Fig. S3. Cross-comparison of the GIWAXS patterns on surface and in bulk for 3D and 3D/2D perovskites, respectively.
      • Fig. S4. Steady-state PL of 3D and 3D/2D perovskite systems.
      • Fig. S5. Hole injection dynamics and band diagram of the 3D/2D perovskite system.
      • Fig. S6. JSC, VOC, FF, and PCE distributions of 50 devices, in which 25 devices are 3D/2D PSCs and 25 are 3D PSCs.
      • Fig. S7. Impedance spectroscopy and capacitance measurement of 3D and 3D/2D PSCs.
      • Fig. S8. Water and humidity resistance of 3D/2D and 3D PSCs.
      • Fig. S9. Image of water droplet on the surface of pure 2D (FEAI)2PbI4 perovskite films.
      • Fig. S10. Stability of a 3D/2D PSC and a 3D PSC at an elevated temperature.

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