Improved Photovoltaic Efficiency and Amplified Photocurrent Generation in Mesoporous n = 1 Two-Dimensional Lead-Iodide Perovskite Solar Cells

Febriansyah, B., Koh, T.M., Lekina, Y. , Jamaludin, N.F., Bruno, A., Ganguly, R., Shen, Z.X., Mhaisalkar, S.G. and England, Jason (2019) Improved Photovoltaic Efficiency and Amplified Photocurrent Generation in Mesoporous n = 1 Two-Dimensional Lead-Iodide Perovskite Solar Cells. Chemistry of Materials, 31 (3). pp. 890-898. ISSN 0897-4756

Full content URL: https://doi.org/10.1021/acs.chemmater.8b04064

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Improved Photovoltaic Efficiency and Amplified Photocurrent Generation in Mesoporous n = 1 Two-Dimensional Lead-Iodide Perovskite Solar Cells
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Abstract

We utilized two organic dications containing, respectively, a pyridinium and an imidazolium core to construct new n = 1 (where n refers to the number of contiguous two-dimensional (2D) inorganic layers, i.e., not separated by organic cations) 2D lead-iodide perovskites 1 and 2. The former material exhibits a (100)- and the latter a very rare 3 � 3 (110)-structural type. Compared with primary ammonium functionality, their constituent ring-centered positive charges have lower charge density. As a result, PbI 6 4- interoctahedral distortions of the inorganic lattice in 1 and 2 are reduced (Pb-I-Pb bond angles are as high as 166° and 174°, respectively). This results in bathochromically shifted optical features. In addition, the compact nature of the dications produces extremely short lead-iodide sheet separations, with respective iodide-iodide (I···I) distances as small as 4.149 and 4.278 à . These are among the shortest separations of adjacent lead-iodide layers ever reported for such materials. When crystallized as thin films on top of substrates, the resulting 2D perovskite layers do not adopt a regular growth direction parallel to the surface. Instead, the crystallites grow with no fixed orientation. As a consequence of their proximate inorganic distances and unusual crystallization tendencies, the resulting 2D perovskites exhibit low excitonic activation energies (93.59 and 96.53 meV, respectively), enhanced photoconductivity in solar cells, and unprecedented incident photon-to-current conversion rates of up to 60%. More importantly, mesoporous 2D layered perovskite solar cells with power conversion efficiencies of 1.43 and 1.83% were achieved for 1 and 2, respectively. These are the highest values obtained thus far for pure n = 1 lead-iodide perovskites and more than 20 times higher than those obtained for materials templated by more conventional cations such as phenylethylammonium (0.08%). Copyright © 2019 American Chemical Society.

Keywords:Activation energy, Efficiency, Iodine compounds, Layered semiconductors, Perovskite, Perovskite solar cells, Positive ions, Solar cells, Solar power generation, Crystallization tendency, Current conversion, Growth directions, Perovskite layers, Photo-voltaic efficiency, Photocurrent generations, Power conversion efficiencies, Two Dimensional (2 D), Lead compounds
Subjects:F Physical Sciences > F131 Crystallography
F Physical Sciences > F200 Materials Science
F Physical Sciences > F120 Inorganic Chemistry
F Physical Sciences > F360 Optical Physics
Divisions:College of Science > School of Chemistry
ID Code:51897
Deposited On:04 Oct 2022 08:41

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