Chemical Tailoring of Band Offsets at the Interface of ZnSe-CdS Heterostructures for Delocalized Photoexcited Charge Carriers

Amit Dalui, Arup Chakraborty, Umamahesh Thupakula, Ali Hossain Khan, Sucheta Sengupta, Biswarup Satpati, D. D. Sarma, Indra Dasgupta, Somobrata Acharya

Research output: Contribution to journalArticlepeer-review

17 Scopus citations

Abstract

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.

Original languageEnglish
Pages (from-to)10118-10128
Number of pages11
JournalJournal of Physical Chemistry C
Volume120
Issue number19
DOIs
StatePublished - 19 May 2016
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2016 American Chemical Society.

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