Pacific Rim Symposium on Surfaces, Coatings and Interfaces (PacSurf 2016)
    Energy Harvesting & Storage Wednesday Sessions
       Session EH-WeP

Paper EH-WeP12
Surfaces And Interfaces Of Methylammonium Lead Halide Perovskite/ Graphene Oxide Films Studied By Spectroscopy

Wednesday, December 14, 2016, 4:00 pm, Room Mauka

Session: Energy Harvesting & Storage Poster Session
Presenter: Muge Acik, Argonne National Laboratory, USA
Authors: M.A. Acik, Argonne National Laboratory, USA
S.B. Darling, Argonne National Laboratory, USA
Correspondent: Click to Email

Power conversion efficiency in perovskite-based solar cells has recently improved to ≥20%, however, there is insufficient understanding of the underlying optoelectronic device function. Among all perovskite materials as candidates for the light harvesters in such solar devices, organolead halide perovskites, MAPbX3 (X=I, Br, Cl), have stood out with their outstanding optoelectronic properties such as tunable bandgaps, long electron-hole diffusion length and high electron/hole mobility. Indeed, replacement of ETL/HTL with graphene-derived materials (graphene oxide, reduced graphene oxide, n/p-doped graphene, etc.) has emerged as a pathway to improve device performance. Nevertheless, unclear film growth, nucleation and degradation mechanisms at the graphene/perovskite hybrid interfaces require understanding of interfacial mechanisms during perovskite growth. Moreover, graphene/perovskite structure-property relationships are not well understood due to unclear chemistry/poor characterization at the interfaces of ETL/perovskite/HTL hybrids. To explore interfacial working mechanisms and perovskite film formation in graphene-derived perovskite solar cells, we performed variable temperature (≤600°C) in situ spectroscopy (infrared absorption, micro-Raman, UV-vis-NIR, x-ray photoelectron and luminescence), and ex situ XRD, SEM, TEM, and AFM for film morphology studies. Our studies targeted perovskite/graphene interfaces and perovskite growth mechanisms to overcome detrimental effects of stability factors such as incomplete lead precursor conversion, inconsistent crystallite formation/film uniformity, and weak cation-anion-solvent coordination. Effect of film thickness, stoichiometry control, underlayer/overlayer composition, and perovskite growth temperature were optimized. To address film scalability and stability, we studied opto-thermal changes in reduced graphene/graphite oxide (RGO) upon halide-based (CH3NH3PbI3, CH3NH3PbBr3, CH3NH3PbCl3) perovskite deposition, and performed spectroscopic analysis derived from the intensity and peak areas of perovskite vibrational modes of C-H (~2800-3200 cm-1) and N-H (~2000-2800 cm-1). Controlled perovskite formation was achieved at room temperature for bromide/chloride-based perovskites resulting improved chemical stability with heat (vs. iodide derivative). Poor perovskite formation was monitored on RGO resulting in film degradation in air (O2, H2O) by in situ characterization. (1) M Acik, SB Darling. J. Mater. Chem. A (2016) 4, 6185-6235. (2) J Gong, SB Darling, F You, Energy Environ. Sci. (2015) 8, 1953-1968. (3) M Acik, G Lee, C Mattevi, M Chhowalla, K Cho, YJ Chabal. Nature Mater. (2010) 9 (10), 840-845.

Use of the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The abstract has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. Office of Science User Facility under Contract No. DE-AC02-06CH11357. M.A. also acknowledges support from the Joseph Katz Named Fellowship at Argonne National Laboratory.