Evolving Stark Effect During Growth of Perovskite Nanocrystals Measured Using Transient Absorption

Methylammonium lead triiodide (MAPbI3) nanocrystals (NCs) are emerging materials for a range of optoelectronic applications. Photophysical characterization is typically limited to structurally stable NCs owing to the long timescales required for many spectroscopies, preventing the accurate measureme...

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Published inFrontiers in chemistry Vol. 8; p. 585853
Main Authors Sadighian, James C., Wilson, Kelly S., Crawford, Michael L., Wong, Cathy Y.
Format Journal Article
LanguageEnglish
Published Frontiers Media S.A 15.10.2020
Subjects
Chemistry
nanocrystals
perovskite
spectroscopy
surface
transient absorption
ultrafast
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Summary:Methylammonium lead triiodide (MAPbI3) nanocrystals (NCs) are emerging materials for a range of optoelectronic applications. Photophysical characterization is typically limited to structurally stable NCs owing to the long timescales required for many spectroscopies, preventing the accurate measurement of NCs during growth. This is a particular challenge for non-linear spectroscopies such as transient absorption. Here we report on the use of a novel single-shot transient absorption (SSTA) spectrometer to study MAPbI3 NCs as they grow. Comparing the transient spectra to derivatives of the linear absorbance reveals that photogenerated charge carriers become localized at surface trap states during NC growth, inducing a TA lineshape characteristic of the Stark effect. Observation of this Stark signal shows that the contribution of trapped carriers to the TA signal declines as growth continues, supporting a growth mechanism with increased surface ligation toward the end of NC growth. This work opens the door to the application of time-resolved spectroscopies to NCs in situ, during their synthesis, to provide greater insight into their growth mechanisms and the evolution of their photophysical properties.
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Edited by: Rene A. Nome, State University of Campinas, Brazil
Reviewed by: Arkaprabha Konar, Kent State University, United States; Minsu Jung, Dong-Eui University, South Korea
This article was submitted to Physical Chemistry and Chemical Physics, a section of the journal Frontiers in Chemistry
ISSN:2296-2646
2296-2646
DOI:10.3389/fchem.2020.585853