Direct observation of charge transfer between molecular heterojunctions based on inorganic semiconductor clusters.

Chemical Science
Chaozhuang XueTao Wu

Abstract

A deep understanding of the dynamics of photogenerated charge carriers is extremely important for promoting their germination in semiconductors to enhance the efficiency of solar energy conversion. In contrast to that of organic molecular heterojunctions (which are widely employed in organic solar cells), the charge transfer dynamics of purely inorganic molecular heterojunctions remains unexplored. Herein, we reveal the dynamics of charge transfer between inorganic semiconductor molecular heteroclusters by selecting a group of open-framework metal chalcogenides as unique structure models constructed from supertetrahedral T3-InS ([In10S20]) and T4-MInS ([M4In16S35], M = Mn or Fe) clusters. The staggered band gap alignment in T3-T4-MInS molecular heterojunctions enables the photogenerated charge carriers to be directionally transferred from T3-InS clusters to adjacent T4-MInS clusters upon irradiation or application of an external electric field. The simultaneous independence of and interactions between such two heteroclusters are investigated by theoretical calculations, steady- and transient-state absorption/photoluminescence spectroscopy, and surface photovoltage analysis. Moreover, the dynamics of cluster-to-cluster-to-dopant...Continue Reading

References

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Methods Mentioned

BETA
X-ray

Software Mentioned

SHELXL
SHELXS
INCAR
Vienna ab initio simulation packages ( VASP )

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