Graphite-Based Localized Heating Technique for Growing Large Area Methylammonium Lead Bromide Single Crystalline Perovskite Wafers and Their Charge Transfer Characteristics

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Abstract
Development of a reproducible technique to grow large area single crystalline perovskite wafers is an open research gap in the field of single crystalline perovskite solar cells. A graphite-based localized heating technique for growing large area methylammonium lead bromide (CH3NH3PbBr3; MAPBr) single crystalline thin film (SCTF) on different buffer layers, such as glass/indium doped tin oxide (ITO), glass/ITO/poly(triaryl amine) (PTAA), and glancing angle deposition (GLAD) coated glass/ITO/TiO2 substrates is reported, and their charge transport properties are discussed. It is observed that the localized heating technique can confine the supersaturation of the precursor mainly to the center of the substrate, leading to a restricted number of nucleations within a specific area on the substrate. Here, such 2-3 seed crystals obtained initially are allowed to grow to a larger size of up to 65 mm2. The X-ray diffraction (XRD) analysis indicated that the large area SCTF is an actual single crystal and not a heterogeneous group of small crystals merged together with a crystallinity index (CI) of 92.60 ± 0.11% which was comparable to that of the bulk single crystal (97.74 ± 0.47%). The atomic force microscopy (AFM) image depicted a smooth SCTF surface (R a = 4.37 ± 0.01 nm), and the wave-like pattern is attributed to the substrate morphology, implying that the topography of the substrate plays a crucial role in obtaining a planar SCTF. The XRD, UV-visible, photoluminescence (PL), Raman, and FTIR spectra analyses revealed that the large area SCTF is phase pure and free of residual impurities. The charge injection characteristics of the SCTFs grown on different buffer layers were investigated using PL emission (PLE) and PL decay analyses. The decrease in the PLE intensity for the SCTFs grown on PTAA and TiO2 substrates implied exciton quenching behavior, indicating the injection of the photogenerated charge carriers into the charge transfer layers (CTLs). The decrease of the fast decay component from τ1 = 4.77 ± 0.18 ns for glass to τ1 = 3.32 ± 0.07 ns for TiO2 and τ1 = 3.15 ± 0.33 ns for PTAA is ascribed to the interfacial recombination of the charges accumulated at the CTL/perovskite interface. These results propose that the localized heating technique can be employed for growing large area single crystalline perovskite wafers for optoelectronic and photovoltaic device applications.
Funding Information
  • Indo-French Centre for the Promotion of Advanced Research (6708-1)

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