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On the Origins of the Stokes Shift in PbS Quantum Dots: Impact of Polydispersity, Ligands and Defects Yun Liu, Donghun Kim, Owen P. Morris, David Zhitomirsky, and Jeffrey C. Grossman ACS Nano, Just Accepted Manuscript • DOI: 10.1021/acsnano.8b00132 • Publication Date (Web): 07 Mar 2018 Downloaded from http://pubs.acs.org on March 7, 2018
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ACS Nano
On the Origins of the Stokes Shift in PbS Quantum Dots: Impact of Polydispersity, Ligands and Defects Yun Liu1*, Donghun Kim2*, Owen P. Morris1, David Zhitomirsky1, Jeffrey C. Grossman1† 1
Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA. 2 Computational Science Research Center, Korea Institute of Science and Technology, Seoul 02792, Korea *Equal Contribution †Correspondence to:
[email protected] Abstract Understanding the origins of the excessive Stokes shift in the lead chalcogenides family of colloidal quantum dots (CQDs) is of great importance at both the fundamental and applied levels; however, our current understanding is far from satisfactory. Here, utilizing a combination of ab initio computations, and UV/vis and photoluminescence measurements, we investigated the contributions to the Stokes shift from polydispersity, ligands, and defects in PbS CQDs. The key results are as follows: (1) The size and energetic disorder of a polydisperse CQD film increase the Stokes shift by 20 to 50 meV compared to that of an isolated CQD; (2) Franck-Condon (FC) shifts increase as the electronegativities of the ligands increase, but the variations are small (
