Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 120, Issue 19, Pages 10118-10128Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.6b00986
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Funding
- SERB, DST India [EMR/2014/000664]
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Monocomponent quantum dots (QDs) possess limited electron-hole delocalization capacity upon photoexcitation that suppresses the efficiency of photoenergy harvesting devices. Type II heterostructures offer band offsets at conduction and valence bands depending upon the band gaps of the constituent QDs which largely depend on their sizes. Hence, by keeping the size of one constituent QD fixed while varying the size of the other QD selectively, the band offsets at the interface can be engineered selectively. We report on the tuning of band offsets by synthesizing component size modulated heterostructures composed of a fixed sized ZnSe QD and size tuned CdS QDs with variable band gaps. The resultant heterostructures show spontaneous charge carrier separation across the interface upon photoexcitation depending on the extent of band offsets. Formation mechanism, epitaxial relationship, and the intrinsic nature of interface of the heterostructures are investigated. Experimental results are corroborated with ab initio electronic structure calculations based on density functional theory. Spontaneous charge carrier delocalization across the interface depends on the magnitude of band offsets, which facilitates fabrication of QD sensitized solar cells (QDSSCs). Improved device performances of QDSSCs in comparison to the limited photon-to-current conversion efficiencies of monocomponent QDs demonstrates the significance of band offsets for natural charge carrier separation.
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