In situ recombination junction between p-Si and TiO2 enables high-efficiency monolithic perovskite/Si tandem cells by Heping Shen, Stefan T. Omelchenko,

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Presentation transcript:

In situ recombination junction between p-Si and TiO2 enables high-efficiency monolithic perovskite/Si tandem cells by Heping Shen, Stefan T. Omelchenko, Daniel A. Jacobs, Sisir Yalamanchili, Yimao Wan, Di Yan, Pheng Phang, The Duong, Yiliang Wu, Yanting Yin, Christian Samundsett, Jun Peng, Nandi Wu, Thomas P. White, Gunther G. Andersson, Nathan S. Lewis, and Kylie R. Catchpole Science Volume 4(12):eaau9711 December 14, 2018 Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 1 Schematic illustration and morphological characterizations of the interlayer-free monolithic perovskite/Si tandem solar cell. Schematic illustration and morphological characterizations of the interlayer-free monolithic perovskite/Si tandem solar cell. (A) Schematic of the interlayer-free monolithic perovskite/crystalline-silicon (c-Si) tandem solar cell (not to scale). Initial tests were carried out on homojunction Si cells with Spiro-OMeTAD (Spiro) as the top perovskite contact; however, our best performance was obtained with polysilicon (poly-Si) bottom cells and PTAA {poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine]} as the top hole-selective layer. (B) Cross-sectional SEM image of the tandem device based on a Si homojunction subcell from the top surface to the p+-Si layer [Spiro-OMeTAD is used as a hole transport material (HTM)]. The antireflection layer was not included because of the large thickness of ~1 mm. (C) Scanning transmission electron microscopy (STEM) bright-field (BF) image, and (D) high-resolution STEM BF image of the TiO2/p+-Si interface. Heping Shen et al. Sci Adv 2018;4:eaau9711 Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 2 Photovoltaic performance and spectral response of the interlayer-free monolithic perovskite/Si tandem solar cell. Photovoltaic performance and spectral response of the interlayer-free monolithic perovskite/Si tandem solar cell. (A) J-V behavior of the proof-of-concept tandem device with both reverse and forward scanning at 0.05 V s−1 based on heterojunction poly-Si subcell. (B) Absorbance (1–reflectance) of the tandem device (gray shading), external quantum efficiency (EQE) of the perovskite top cell (blue), and EQE of the c-Si bottom subcell (red). Heping Shen et al. Sci Adv 2018;4:eaau9711 Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 3 Contact behavior and simulated band diagram of TiO2/p+-Si interfaces. Contact behavior and simulated band diagram of TiO2/p+-Si interfaces. (A) Schematic of the structure used for measuring contact resistivity. (B) Comparison of the J-V behavior of ITO/p+-Si and various TiO2/p+-Si structures before and after annealing at 400°C in air. TiCl4-ALD TiO2 listed here is deposited with a reactor chamber temperature of 75°C. (C) Simulated band diagram of the TiO2/p+-Si at equilibrium assuming n-type doping of 5 × 1018 cm−3 on TiO2 and 1019 cm−3 for p+-Si (appropriate for our test structure with TDMAT TiO2; see table S3). The unknown interfacial energy gap Δ is shown here for illustrative purposes as 600 meV, which falls within the range of reported measurements (31). Both mechanisms of direct- and tunneling-assisted capture by interfacial density of states (DoS) are shown. Heping Shen et al. Sci Adv 2018;4:eaau9711 Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 4 Mechanism understanding of low contact resistivity of TiO2/p+-Si interfaces and simulated band diagram of the full tandem device. Mechanism understanding of low contact resistivity of TiO2/p+-Si interfaces and simulated band diagram of the full tandem device. (A) Simulated J-V behavior for varying interfacial gaps Δ. A single neutral midgap SRH defect was included with Sn = Sp = 105 cm s−1. The dashed curves are computed with tunneling to defects included. (B) Simulated small voltage resistivity with the TiO2 donor density fixed at 1018 cm−3 and variable p-Si acceptor doping, NA. Measurements are included as data points in red. Calculations for neutral (dashed line), acceptor type (dotted-dashed line), and donor type (solid lines) are shown to demonstrate the important effect of defect charge on the interfacial carrier balance. (C) Simulated band diagram of the full tandem device based on a homojunction Si subcell with high work-function cp-TiO2 at illuminated open circuit. The inset depicts the two important energetic offsets Δ and δ, respectively, defined as the valence-to-conduction band offset at the TiO2-Si interface and the difference in work functions between our solution-processed ms-TiO2 layer and that of the ALD compact layer. Heping Shen et al. Sci Adv 2018;4:eaau9711 Copyright © 2018 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).