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Enhancing the solar energy conversion efficiency of solution-deposited Bi2S3 thin films by annealing in sulfur vapor at elevated temperature

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Abstract

Bi2S3 is a non-toxic n-type semiconductor, which has been commonly synthesized in the form of quantum dots or nanocrystalline films by solution deposition methods. Despite a favorable optical band gap of ∼1.3 eV, such films have not achieved high solar energy conversion efficiencies to date. We hypothesize that this is in part due to the presence of sulfur vacancies that, according to our density functional theory calculations, form a deep trap state in the band gap of Bi2S3, which can act as a strong recombination channel for photoexcited charges. Here, we report a microcrystalline Bi2S3 thin-film synthesized by annealing solution-deposited nanocrystalline Bi2S3 in a sulfur vapor environment at 445 °C, which simultaneously increases the grain size and phase purity of Bi2S3, fills in sulfur vacancies, and improves optical absorption. Time-resolved terahertz spectroscopy (TRTS) reveals that sulfur annealing increases the photoexcited carrier lifetime from sub-picosecond to ∼30 picoseconds, while the internal quantum efficiency of a photoelectrochemical solar cell device is increased 4-fold from ∼10% to ∼40%. In addition, TRTS reveals that the intra-grain carrier mobility in the sulfur-annealed films is ∼165 cm2 V−1 s−1 and the long-range mobility is ∼111 cm2 V−1 s−1 at short times, indicating that carriers are able to hop across grain boundaries. These results indicate that annealing in sulfur vapor can produce simultaneously high light absorption and charge separation efficiencies by achieving carrier diffusion length that is comparable to the light absorption depth, leading to high solar energy conversion efficiencies in Bi2S3.

Graphical abstract: Enhancing the solar energy conversion efficiency of solution-deposited Bi2S3 thin films by annealing in sulfur vapor at elevated temperature

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Publication details

The article was received on 14 Aug 2017, accepted on 24 Sep 2017 and first published on 26 Sep 2017


Article type: Paper
DOI: 10.1039/C7SE00398F
Citation: Sustainable Energy Fuels, 2017, Advance Article
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    Enhancing the solar energy conversion efficiency of solution-deposited Bi2S3 thin films by annealing in sulfur vapor at elevated temperature

    Z. Zhu, S. K. Iyemperumal, K. Kushnir, A. D. Carl, L. Zhou, D. R. Brodeur, Ronald L. Grimm, L. V. Titova, N. A. Deskins and P. M. Rao, Sustainable Energy Fuels, 2017, Advance Article , DOI: 10.1039/C7SE00398F

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