Strong Photocurrent from Two-Dimensional Excitons in Solution-Processed Stacked Perovskite Semiconductor Sheets

Room-temperature photocurrent measurements in two-dimensional (2D) inorganic-organic perovskite devices reveal that excitons strongly contribute to the photocurrents despite possessing binding energies over 10 times larger than the thermal energies. The p-type (C₆H₉C₂H₄NH₃)₂PbI₄ liberates photocarriers at metallic Schottky aluminum contacts, but incorporating electron- and hole-transport layers enhances the extracted photocurrents by 100-fold. A further 10-fold gain is found when TiO₂ nanoparticles are directly integrated into the perovskite layers, although the 2D exciton semiconducting layers are not significantly disrupted. These results show that strong excitonic materials may be useful as photovoltaic materials despite high exciton binding energies and suggest mechanisms to better understand the photovoltaic properties of the related three-dimensional perovskites.This work was supported by EPSRC Grants EP/K028510/1, EP/G060649/1, EP/G037221/1, EP/H007024/1, EP/L027151/1, and EP/L015978/1, the Cambridge NanoDTC, and ERC LINASS 320503

In situ intercalation dynamics in inorganic-organic layered perovskite thin films

The properties of layered inorganic semiconductors can be manipulated by the insertion of foreign molecular species via a process known as intercalation. In the present study, we investigate the phenomenon of organic moiety (R-NH3I) intercalation in layered metal-halide (PbI 2)-based inorganic semiconductors, leading to the formation of inorganic-organic (IO) perovskites [(R-NH3)2PbI 4]. During this intercalation strong resonant exciton optical transitions are created, enabling study of the dynamics of this process. Simultaneous in situ photoluminescence (PL) and transmission measurements are used to track the structural and exciton evolution. On the basis of the experimental observations, a model is proposed which explains the process of IO perovskite formation during intercalation of the organic moiety through the inorganic semiconductor layers. The interplay between precursor film thickness and organic solution concentration/solvent highlights the role of van der Waals interactions between the layers, as well as the need for maintaining stoichiometry during intercalation. Nucleation and growth occurring during intercalation matches a Johnson-Mehl-Avrami-Kolmogorov model, with results fitting both ideal and nonideal cases. © 2014 American Chemical Society

Strong Photocurrent from Two-Dimensional Excitons in Solution-Processed Stacked Perovskite Semiconductor Sheets

Room-temperature photocurrent measurements in two-dimensional (2D) inorganic-organic perovskite devices reveal that excitons strongly contribute to the photocurrents despite possessing binding energies over 10 times larger than the thermal energies. The p-type (C₆H₉C₂H₄NH₃)₂PbI₄ liberates photocarriers at metallic Schottky aluminum contacts, but incorporating electron- and hole-transport layers enhances the extracted photocurrents by 100-fold. A further 10-fold gain is found when TiO₂ nanoparticles are directly integrated into the perovskite layers, although the 2D exciton semiconducting layers are not significantly disrupted. These results show that strong excitonic materials may be useful as photovoltaic materials despite high exciton binding energies and suggest mechanisms to better understand the photovoltaic properties of the related three-dimensional perovskites.This work was supported by EPSRC Grants EP/K028510/1, EP/G060649/1, EP/G037221/1, EP/H007024/1, EP/L027151/1, and EP/L015978/1, the Cambridge NanoDTC, and ERC LINASS 320503

Strong Photocurrent from Two-Dimensional Excitons in Solution-Processed Stacked Perovskite Semiconductor Sheets

Room-temperature photocurrent measurements in two-dimensional (2D) inorganic-organic perovskite devices reveal that excitons strongly contribute to the photocurrents despite possessing binding energies over 10 times larger than the thermal energies. The p-type (C₆H₉C₂H₄NH₃)₂PbI₄ liberates photocarriers at metallic Schottky aluminum contacts, but incorporating electron- and hole-transport layers enhances the extracted photocurrents by 100-fold. A further 10-fold gain is found when TiO₂ nanoparticles are directly integrated into the perovskite layers, although the 2D exciton semiconducting layers are not significantly disrupted. These results show that strong excitonic materials may be useful as photovoltaic materials despite high exciton binding energies and suggest mechanisms to better understand the photovoltaic properties of the related three-dimensional perovskites