ABSTRACT
We report on utilizing free-standing hybrid perylenediimide/carbon nanotube (PDI/CNT) films fabricated in air as back contacts for fully inorganic perovskite solar cells (glass/FTO/dense TiO2/mesoporous TiO2/CsPbBr3/back electrode). The back contact electrode connection is performed by film transfer rather than by vacuum deposition or by wet processing, allowing the formation of highly homogeneous contacts under ambient conditions. The use of this novel electrode in solar cells based on CsPbBr3 resulted in efficiency of 5.8% without a hole transporting layer; it is significantly improved in comparison to the reference cells with standard gold electrodes. Overall device fabrication can be performed on air, using inexpensive processing methods. The hybrid film electrodes dramatically improve the cell photo-stability under ambient conditions and under real-life operating conditions outdoors. The champion unencapsulated device demonstrated less than 30% efficiency loss over 6 weeks of outdoor aging in Negev desert conditions. The CNT/PDI electrodes offer the combination of fabrication simplicity, unique contacting approach, high efficiency and good operational stability for perovskite photovoltaics.
ABSTRACT
Joint experimental and theoretical work is presented on two quadrupolar D-π-A-π-D chromophores characterized by the same bulky donor (D) group and two different central cores. The first chromophore, a newly synthesized species with a malononitrile-based acceptor (A) group, has a V-shaped structure that makes its absorption spectrum very broad, covering most of the visible region. The second chromophore has a squaraine-based core and therefore a linear structure, as also evinced from its absorption spectra. Both chromophores show an anomalous red shift of the absorption band upon increasing solvent polarity, a feature that is ascribed to the large, bulky structure of the molecules. For these molecules, the basic description of polar solvation in terms of a uniform reaction field fails. Indeed, a simple extension of the model to account for two independent reaction fields associated with the two molecular arms quantitatively reproduces the observed linear absorption and fluorescence as well as fluorescence anisotropy spectra, fully rationalizing their nontrivial dependence on solvent polarity. The model derived from the analysis of linear spectra is adopted to predict nonlinear spectra and specifically hyper-Rayleigh scattering and two-photon absorption spectra. In polar solvents, the V-shaped chromophore is predicted to have a large HRS response in a wide spectral region (approximately 600-1300 nm). Anomalously large and largely solvent-dependent HRS responses for the linear chromophores are ascribed to symmetry lowering induced by polar solvation and amplified in this bulky system by the presence of two reaction fields.
