Research ArticleMATERIALS SCIENCE

A general printing approach for scalable growth of perovskite single-crystal films

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Science Advances  29 Jun 2018:
Vol. 4, no. 6, eaat2390
DOI: 10.1126/sciadv.aat2390
  • Fig. 1 Seed printing of perovskite single-crystal films.

    (A) Schematic illustration of the scalable growth of perovskite single-crystal films. First, perovskite seed stamp is fabricated using an inkjet printing method. Second, the prepared seed stamp is covered on the target substrate with perovskite solution, and perovskite single-crystal films in situ grow as the solvent dries. Taking away the covered stamp, we printed the perovskite single-crystal films on the substrate. Scale bar, 1 mm. (B) Synchrotron-radiated single-crystal XRD photograph of the perovskite film on quartz glass by rotating the incident x-ray angle of ±22.5°. All the diffraction rings belonged to the quartz glass substrate. (C) XRD pattern for the perovskite single-crystal film. a.u., arbitrary units. (D) AFM profile of the perovskite single-crystal film surface.

  • Fig. 2 The inhibition of random nucleation and film growth.

    (A) Optical image of the patterned perovskite seeds for the growth of perovskite single-crystal films. Scale bar, 100 μm. (B) Suppression ability of random nucleation as a function of the distance of seeds. The suppression ability of random nucleation was defined as N0/N, where N0 is the number of the origin perovskite seeds (N0 = 100) and N is the total number of crystals within the seed regions after a crystallization time of 30 min. (C) Photo of perovskite seeds with the distance l = 0.5 mm growing on quartz glass for 24 hours. It can be observed that the outside films are larger than the inside ones, and no excrescent nucleation exists between the seeds. Scale bar, 100 μm. (D) Thickness of perovskite single-crystal films on quartz glass as a function of the seed size, which is controlled by the concentration of printed perovskite solution. It shows that the perovskite single-crystal film thickness approximately linearly increases with the seed size and that the thickness of the perovskite single-crystal films can be flexibly tuned by the origin seed size from hundreds of nanometers to more than ten micrometers.

  • Fig. 3 Optical and trap density property.

    (A) Steady-state micro-area absorbance and PL of the perovskite single-crystal films. PL excitation wavelength is 405 nm. (B) Fluorescence microscopy image of the perovskite single-crystal film. The uniform luminescence of the film verifies its high quality without visible defects. Scale bar, 50 μm. (C) Current-voltage trace of perovskite single-crystal films. It shows a linear ohmic region followed by the trap-filled region at VTFL = 0.36 V. The trap density determined by VTFL was calculated as ntrap = 2.6 × 10−10 cm−3. (D) PL time decay trace of the perovskite single-crystal films at 540 nm showing a fast component (τ1 = 43 ns) and a slow component (τ2 = 391 ns).

  • Fig. 4 Printing perovskite single-crystal film on various kinds of substrates.

    Optical microscopy images of the perovskite single-crystal film on (A) glass, (B) quartz glass, and (C) silicon wafer. (D) SEM image of the perovskite single-crystal film on graphene. Optical microscopy images of the perovskite single-crystal film on (E) MoS2, (F) FTO glass, (G) PET film, (H) PI film, and (I) PE film. Scale bars, 50 μm (A to C and E to I) and 5 μm (D).

  • Fig. 5 Scalable fabrication of photodetectors.

    (A) Schematic device structure of the perovskite single-crystal photodetectors. (B) Current-voltage characteristic measured in the dark condition. (C) Current-voltage curve in different incident light intensities. (D) Transient photocurrent of the photodetector (bias, 3 V; λ = 450 nm).

  • Fig. 6 Image sensor based on the perovskite single-crystal film.

    (A) Optical image of electrode arrays on the perovskite single-crystal film. Scale bar, 200 μm. (B) Photocurrent mapping of the perovskite single-crystal film. (C) Optical image of the number 10. Scale bar, 100 μm. (D) Photocurrent intensity profile of the optical image 10.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/6/eaat2390/DC1

    fig. S1. The SEM images of the as-grown perovskite single-crystal film.

    fig. S2. Optical microscopy image and AFM image of the perovskite single-crystal film.

    fig. S3. Synchrotron-radiated single-crystal XRD analysis.

    fig. S4. EDS mappings of the perovskite single-crystal films.

    fig. S5. Powder XRD patterns of the perovskite single-crystal films.

    fig. S6. Optical microscopy images of the seed crystal regions.

    fig. S7. Scalable fabrication of perovskite single-crystal films.

    fig. S8. Perovskite single-crystal film growth process.

    fig. S9. The height profiles of perovskite single-crystal films with different thicknesses.

    fig. S10. Responsivity as a function of incident light intensity.

  • Supplementary Materials

    This PDF file includes:

    • fig. S1. The SEM images of the as-grown perovskite single-crystal film.
    • fig. S2. Optical microscopy image and AFM image of the perovskite single-crystal film.
    • fig. S3. Synchrotron-radiated single-crystal XRD analysis.
    • fig. S4. EDS mappings of the perovskite single-crystal films.
    • fig. S5. Powder XRD patterns of the perovskite single-crystal films.
    • fig. S6. Optical microscopy images of the seed crystal regions.
    • fig. S7. Scalable fabrication of perovskite single-crystal films.
    • fig. S8. Perovskite single-crystal film growth process.
    • fig. S9. The height profiles of perovskite single-crystal films with different thicknesses.
    • fig. S10. Responsivity as a function of incident light intensity.

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