Direct observation of charge transfer between molecular heterojunctions based on inorganic semiconductor clusters,Chemical Science

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Direct observation of charge transfer between molecular heterojunctions based on inorganic semiconductor clusters
Chemical Science ( IF 7.6 ) Pub Date : 2020-03-23 , DOI: 10.1039/d0sc00458h
Chaozhuang Xue _{1,

2,

3,

4} , Xing Fan _{2,

4,

5,

6,

7} , Jiaxu Zhang _{1,

2,

3,

4} , Dandan Hu _{1,

2,

3,

4} , Xiao-Li Wang _{1,

2,

3,

4} , Xiang Wang _{1,

2,

3,

4} , Rui Zhou _{1,

2,

3,

4} , Haiping Lin _{2,

4,

5,

6,

7} , Youyong Li _{2,

4,

5,

6,

7} , Dong-Sheng Li _{8,

9,

10,

11,

12} , Xiao Wei _{4,

13,

14,

15} , Daoyuan Zheng _{4,

16,

17,

18,

19} , Yang Yang _{4,

16,

17,

18,

19} , Keli Han _{4,

16,

17,

18,

19} , Tao Wu _{1,

2,

3,

4}

Affiliation

College of Chemistry, Chemical Engineering and Materials Science
Soochow University
Suzhou 215123
China
Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices
Institute of Functional Nano & Soft Materials (FUNSOM)
Suzhou
Hubei Provincial Collaborative Innovation Center for New Energy Microgrid
Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials
College of Materials and Chemical Engineering
China Three Gorges University
Yichang 443002
School of Chemistry and Chemical Engineering
Shanghai Jiao Tong University
Shanghai 200240
State Key Laboratory of Molecular Reaction Dynamics
Dalian Institute of Chemical Physics
Chinese Academy of Science
Dalian 116023

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 photogenerated charge transfer is deliberately elucidated. Thus, this work demonstrates the direct observation of charge transfer between molecular heterojunctions based on purely inorganic semiconductor clusters and is expected to promote the development of cluster-based semiconductors for solar cells.

中文翻译：

直接观察基于无机半导体簇的分子异质结之间的电荷转移

对光生电荷载流子动力学的深刻理解对于促进它们在半导体中的萌发以提高太阳能转换效率非常重要。与有机分子异质结（在有机太阳能电池中广泛使用）相反，纯无机分子异质结的电荷转移动力学仍未探索。在这里，我们通过选择一组开放框架的金属硫族化物作为由超四面体T3-InS（[In ₁₀ S ₂₀ ]）和T4-MInS（[M ₄在₁₆ S ₃₅]，M = Mn或Fe）团簇。T3-T4-MInS中的交错带隙对准分子异质结使光生电荷载流子在辐照或施加外部电场时能从T3-InS簇定向转移到相邻的T4-MInS簇。通过理论计算，稳态和瞬态吸收/光致发光光谱以及表面光电压分析，研究了这两个杂簇的同时独立性和相互作用。此外，刻意阐明了簇到簇到掺杂剂的光生电荷转移的动力学。因此，这项工作证明了直接观察基于纯无机半导体簇的分子异质结之间的电荷转移，并有望促进用于太阳能电池的基于簇的半导体的发展。

更新日期：2020-03-23

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