| AVS 64th International Symposium & Exhibition | |
| Nanometer-scale Science and Technology Division | Wednesday Sessions |
| Session NS+SS+SU-WeM |
| Session: | Nanotechnology for Renewable Energy |
| Presenter: | Muge Acik, Argonne National Laboratory |
| Authors: | M.A. Acik, Argonne National Laboratory G. Lee, Ulsan National Institute of Science and Technology, Korea R.A. Rosenberg, Argonne National Laboratory |
| Correspondent: | Click to Email |
High power conversion efficiency of perovskite-based solar cells offers promise for low-cost and scalable production of renewable energy. Hybrid organic-inorganic methylammonium lead halides, MAPbX3 (X=I, Br, Cl)/mixed-halides (I3-xClx, I3-xBrx) have been reported as light harvesting layers with tunable bandgaps, long electron-hole diffusion lengths and high electron/hole mobility. Nevertheless, halide-based perovskites require in situ investigation for film growth mechanisms to overcome detrimental effects of incomplete lead precursor conversion, inconsistent crystallite formation/film uniformity, and weak cation-anion-solvent coordination (1). Graphene-derived hybrids has recently emerged as an ETL/HTL replacement in these devices. Graphene/perovskite structure-property relationships are, however, not well understood due to unclear chemistry at the ETL/perovskite/HTL interfaces (2). Moreover, effect of film thickness, lead content, stoichiometry control, and overlayer/underlayer morphology/composition ought to be examined for better charge transport at the graphene/perovskite interfaces. Stability factors also need to be studied for charge mechanisms to unravel device performance challenges. Indeed, underlayer ETLs (TiO2/Al2O3) and overlayer HTLs (spiro-OMeTAD) were rarely studied with graphene. To address scalability and stability issues, we investigated degradation, nucleation and growth mechanisms in reduced graphene/graphite oxide (RGO) upon halide-based (I, Cl, Br) perovskite deposition. Chemical interactions were interpreted at perovskite/RGO interfaces for the grain size, orientation, boundaries, and surface/bulk effects using variable-temperature (≤600°C, Ar(g)) in situ spectroscopy (infrared absorption and micro-Raman). Controlled perovskite formation was achieved at room temperature for bromide-based perovskites resulting in improved chemical stability (vs. iodide/chloride derivative). Perovskite decomposition was observed at ≥150°C on RGO surfaces. Oxygen-induced chemical reactions occurred at ≤150°C, initiated at room temperature because of precursor interactions forming carbonyls upon perovskite deposition (3), and eliminated hydroxyls reducing GO during perovskite growth. Poor perovskite formation was observed on RGO due to varying electron affinity and reactivity of precursor halides, resulting in film degradation in air (O2, H2O). Film morphology was explored by SEM, XRD, XPS, AFM, and the reaction mechanisms were studied by first principles calculations that bring insights for solar cell design principles.
Acknowledgement
“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.”