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Electronic Structure Modulation of 2D Colloidal CdSe Nanoplatelets by Au25 Clusters for High-Performance Photodetectors
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-08-12 , DOI: 10.1021/acs.jpcc.0c04774 Anusri Medda 1 , Avisek Dutta 1 , Dipankar Bain 1 , Manish Kumar Mohanta 2 , Abir De Sarkar 2 , Amitava Patra 1, 2
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-08-12 , DOI: 10.1021/acs.jpcc.0c04774 Anusri Medda 1 , Avisek Dutta 1 , Dipankar Bain 1 , Manish Kumar Mohanta 2 , Abir De Sarkar 2 , Amitava Patra 1, 2
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The electronic interactions between colloidal two-dimensional (2D) semiconductor nanoplatelets (NPLs) and Au nanoclusters (NCs) remain unexplored, which are decisive for optoelectronic applications. Here, we report the synthesis of heterostructures based on colloidal 2D CdSe NPLs and Au25 NCs and investigate their electronic interactions using density functional theory (DFT) calculations. The steady state, time-resolved photoluminescence, and transient absorption (TA) spectroscopic studies are carried out to understand the charge-transfer dynamics. The replacement of CdSe bands by Au bands in the valence band edge in CdSe NPLs–Au NCs heterostructures attests the charge transfer from the conduction band of CdSe to Au. Ultrafast TA spectroscopy further confirms the electron transfer in the heterostructures, and the faster bleach recovery kinetics is also observed in CdSe NPLs–Au NCs heterostructures. The observed charge transfer from the conduction band of CdSe NPLs to Au NCs has been corroborated by the difference in the orbital composition of the valence band edges between CdSe and Au NCs, as calculated by DFT. Photodetectors fabricated with these heterostructures feature high enhancement in photocurrent (∼350-fold), fast photoresponse (∼200 ms), and high detectivity (∼2.5 × 1011 Jones), which hold promise for the future design of 2D NPL-based materials for optoelectronic applications.
中文翻译：
用于高性能光电探测器的Au 25团簇对2D胶态CdSe纳米片的电子结构调节
胶体二维（2D）半导体纳米片（NPL）和金纳米团簇（NC）之间的电子相互作用仍未开发，这对于光电应用至关重要。在这里，我们报告基于胶体二维CdSe NPL和Au 25的异质结构的合成NC并使用密度泛函理论（DFT）计算研究其电子相互作用。为了了解电荷转移动力学，进行了稳态，时间分辨的光致发光和瞬态吸收（TA）光谱研究。CdSe NPLs-Au NCs异质结构的价带边缘中的Au谱带替换了CdSe谱带，证明了电荷从CdSe的导带转移到Au。超快TA光谱进一步证实了异质结构中的电子转移，并且在CdSe NPLs-Au NCs异质结构中还观察到了更快的漂白回收动力学。由DFT计算得出，CdSe和Au NCs之间的价带边缘的轨道组成存在差异，这证实了从CdSe NPLs的导带到Au NCs的电荷转移。11 Jones），这为光电子应用中基于2D NPL的材料的未来设计提供了希望。
更新日期：2020-09-10
中文翻译：
用于高性能光电探测器的Au 25团簇对2D胶态CdSe纳米片的电子结构调节
胶体二维（2D）半导体纳米片（NPL）和金纳米团簇（NC）之间的电子相互作用仍未开发，这对于光电应用至关重要。在这里，我们报告基于胶体二维CdSe NPL和Au 25的异质结构的合成NC并使用密度泛函理论（DFT）计算研究其电子相互作用。为了了解电荷转移动力学，进行了稳态，时间分辨的光致发光和瞬态吸收（TA）光谱研究。CdSe NPLs-Au NCs异质结构的价带边缘中的Au谱带替换了CdSe谱带，证明了电荷从CdSe的导带转移到Au。超快TA光谱进一步证实了异质结构中的电子转移，并且在CdSe NPLs-Au NCs异质结构中还观察到了更快的漂白回收动力学。由DFT计算得出，CdSe和Au NCs之间的价带边缘的轨道组成存在差异，这证实了从CdSe NPLs的导带到Au NCs的电荷转移。11 Jones），这为光电子应用中基于2D NPL的材料的未来设计提供了希望。
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