Fabian, DM; Ganose, AM; Ziller, JW; Scanlon, DO; Beard, MC; Ardo, S; (2019) Influence of One Specific Carbon–Carbon Bond on the Quality, Stability, and Photovoltaic Performance of Hybrid Organic–Inorganic Bismuth Iodide Materials. ACS Applied Energy Materials , 2 (3) pp. 1579-1587. 10.1021/acsaem.8b01809.

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Abstract

Hybrid organic–inorganic halide perovskites are promising materials for thin-film solar cells. However, the toxicity and instability of best-in-class lead–halide perovskite materials make them nonideal. To combat these issues, we replaced lead with bismuth and explored the sensitivity of these new lead-free materials to the valency and bonding of their cationic organic groups. Specifically, we synthesized and characterized the materials properties and photophysical properties of hexane-1,6-diammonium bismuth pentaiodide ((HDA^{2+}Bil_{5}) and compared them to an analogue containing a more volatile organic group with half the number of carbon and nitrogen atoms in the form of n-propylammonium ((PA+)_{x}Bil_{3+x}, where 1<x<3). The full crystallographic structures of (HDA^{2+})Bil_{5} and (PA^{+})_{x}Bil_{3+x} were resolved by single-crystal X-ray diffraction. (HDA^{2+})Bil_{5} was shown to be pure-phase and have a one-dimensional structure, whereas (PA^{+})_{x}Bil_{3+x} was shown to be a mix of one-dimensional and zero-dimensional phases. Structures of the materials were confirmed by synchrotron X-ray diffraction of powders. Both (HDA^{2+})Bil_{5} and (PA^{+})_{x}Bil_{3+x} exhibit steady-state photoluminescence at room temperature. Density functional theory calculations of (HDA^{2+})Bil_{5} predict electronic absorption features and a ∼2 eV bandgap that are consistent with those observed experimentally. Structure–property relationships of the materials were examined, and moisture tolerance and film quality were found to be superior for dication-containing (HDA^{2+})Bil_{5} in relation to monocation-containing (PA^{+})_{x}Bil_{3+x}. We hypothesize that these trends are in part due to a molecular bridging effect enabled by the presence of the dicationic hexanediammonium groups in (HDA^{2+})Bil_{5}. Solar cells fabricated using (HDA^{2+})Bil_{5} as the photoactive layer exhibited photovoltaic action while those containing (PA^{+})_{x}Bil_{3+x} did not, suggesting that organic dicationic groups are beneficial to light-absorber morphology and ultimately solar-cell performance.

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