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Electron-hole separation in ferroelectric oxides for efficient photovoltaic responses.


ABSTRACT: Despite their potential to exceed the theoretical Shockley-Queisser limit, ferroelectric photovoltaics (FPVs) have performed inefficiently due to their extremely low photocurrents. Incorporating Bi2FeCrO6 (BFCO) as the light absorber in FPVs has recently led to impressively high and record photocurrents [Nechache R, et al. (2015) Nat Photonics 9:61-67], which has revived the FPV field. However, our understanding of this remarkable phenomenon is far from satisfactory. Here, we use first-principles calculations to determine that such excellent performance mainly lies in the efficient separation of electron-hole (e-h) pairs. We show that photoexcited electrons and holes in BFCO are spatially separated on the Fe and Cr sites, respectively. This separation is much more pronounced in disordered BFCO phases, which adequately explains the observed exceptional PV responses. We further establish a design strategy to discover next-generation FPV materials. By exploring 44 additional Bi-based double-perovskite oxides, we suggest five active-layer materials that offer a combination of strong e-h separations and visible-light absorptions for FPV applications. Our work indicates that charge separation is the most important issue to be addressed for FPVs to compete with conventional devices.

SUBMITTER: Kim D 

PROVIDER: S-EPMC6042087 | biostudies-other | 2018 Jun

REPOSITORIES: biostudies-other

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Electron-hole separation in ferroelectric oxides for efficient photovoltaic responses.

Kim Donghoon D   Han Hyeon H   Lee June Ho JH   Choi Jin Woo JW   Grossman Jeffrey C JC   Jang Hyun Myung HM   Kim Donghun D  

Proceedings of the National Academy of Sciences of the United States of America 20180611 26


Despite their potential to exceed the theoretical Shockley-Queisser limit, ferroelectric photovoltaics (FPVs) have performed inefficiently due to their extremely low photocurrents. Incorporating Bi<sub>2</sub>FeCrO<sub>6</sub> (BFCO) as the light absorber in FPVs has recently led to impressively high and record photocurrents [Nechache R, et al. (2015) <i>Nat Photonics</i> 9:61-67], which has revived the FPV field. However, our understanding of this remarkable phenomenon is far from satisfactory.  ...[more]

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