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Role of Pb2+ Adsorbents on the Opto-Electronic Properties of a CsPbBr3 Nanocrystal: A DFT Study

Published online by Cambridge University Press:  13 June 2019

Aaron Forde ,
Erik Hobbie  and
Dmitri Kilin
Aaron Forde*
Affiliation:
Department of Materials Science and Nanotechnology, North Dakota State University, Fargo, North Dakota58102, United States
Erik Hobbie
Affiliation:
Department of Materials Science and Nanotechnology, North Dakota State University, Fargo, North Dakota58102, United States
Dmitri Kilin
Affiliation:
Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota58102, United States
*
*(Email: Aaron.forde@ndsu.edu)
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Abstract

Fully inorganic lead halide perovskite nanocrystals (NCs) are of interest for photovoltaic and light emitting devices due to optoelectronic properties. Understanding the surface chemistry of these materials is of importance as surface defects can introduce trap-states which reduce their functionality. Here we use Density Functional Theory (DFT) to model surface defects introduced by Pb2+ on a CsPbBr3 NC atomistic model. Two types of defects are studied: (i) an under-coordinated Pb2+ surface atom and (ii) Pb2+ atomic or molecular adsorbents to the NC surface. From the DFT calculations we compute the density of states (DOS) and absorption spectra of the defect models to the pristine fully-passivated NC model. We observe that for the low surface defect regime explored here that neither (i) or (ii) produce trap-states inside of the bandgap and exhibit bright optical absorption for the lowest energy transition. From the models studied, it was found that the Pb2+ atomic absorbent provides broadening of the conduction band edge, which implies chemisorption of Pb2+ to the NC surface. At higher defect densities it would be expected that Pb2+ atomic absorbents would introduce trap-states and degrade the opto-electronic properties of these materials.

Keywords

quantum dotperovskites
Type
Articles
Information
MRS Advances , Volume 4 , Issue 36: Energy and Sustainability , 2019 , pp. 1981 - 1988
Copyright
Copyright © Materials Research Society 2019 

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