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Title: Origin of Photocarrier Losses in Iron Pyrite (FeS2) Nanocubes
Authors: Shukla, Sudhanshu
Xing, Guichuan
Ge, Hu
Prabhakar, Rajiv Ramanujam
Mathew, Sinu
Su, Zhenghua
Nalla, Venkatram
Venkatesan, Thirumalai
Mathews, Nripan
Sritharan, Thirumany
Sum, Tze Chien
Xiong, Qihua
Keywords: Variable range hopping
Transient absorption
Issue Date: 2016
Source: Shukla, S., Xing, G., Ge, H., Prabhakar, R. R., Mathew, S., Su, Z., et al. (2016). Origin of Photocarrier Losses in Iron Pyrite (FeS2) Nanocubes. ACS Nano, 10(4), 4431-4440.
Series/Report no.: ACS Nano
Abstract: Iron pyrite has received significant attention due to its high optical absorption. However, the loss of open circuit voltage (Voc) prevents its further application in photovoltaics. Herein, we have studied the photophysics of pyrite by ultrafast laser spectroscopy to understand fundamental limitation of low Voc by quantifying photocarrier losses in high quality, stoichiometric, and phase pure {100} faceted pyrite nanocubes. We found that fast carrier localization of photoexcited carriers to indirect band edge and shallow trap states is responsible for major carrier loss. Slow relaxation component reflects high density of defects within the band gap which is consistent with the observed Mott-variable range hopping (VRH) conduction from transport measurements. Magnetic measurements strikingly show the magnetic ordering associated with phase inhomogeneity, such as FeS2−δ (0 ≤ δ ≤ 1). This implies that improvement of iron pyrite solar cell performance lies in mitigating the intrinsic defects (such as sulfur vacancies) by blocking the fast carrier localization process. Photocarrier generation and relaxation model is presented by comprehensive analysis. Our results provide insight into possible defects that induce midgap states and facilitate rapid carrier relaxation before collection.
ISSN: 1936-0851
DOI: 10.1021/acsnano.6b00065
Rights: © 2016 American Chemical Society.
Fulltext Permission: none
Fulltext Availability: No Fulltext
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