Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy

Mary Jane Simpson; Benjamin Doughty; Bin Yang; Kai Xiao; Ying Zhong Ma

doi:10.1021/acsphotonics.5b00638

Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy

Mary Jane Simpson, Benjamin Doughty, Bin Yang, Kai Xiao, Ying Zhong Ma

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

Femtosecond transient absorption microscopy is a novel chemical imaging capability with simultaneous high spatial and temporal resolution. Although several powerful data analysis approaches have been developed and successfully applied to separate distinct chemical species in such images, the application of such analysis to distinguish different photoexcited species is rare. In this paper, we demonstrate a combined approach based on phasor and linear decomposition analysis on a microscopic level that allows us to separate the contributions of both the excitons and free charge carriers in the observed transient absorption response of a composite organometallic lead halide perovskite film. We found spatial regions where the transient absorption response was predominately a result of excitons and others where it was predominately due to charge carriers, and regions consisting of signals from both contributors. Quantitative decomposition of the transient absorption response curves further enabled us to reveal the relative contribution of each photoexcitation to the measured response at spatially resolved locations in the film.

Original language	English
Pages (from-to)	434-442
Number of pages	9
Journal	ACS Photonics
Volume	3
Issue number	3
DOIs	https://doi.org/10.1021/acsphotonics.5b00638
State	Published - Mar 16 2016

Funding

M.J.S., B.D., and Y.-Z.M. were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Perovskite sample preparation by B.Y. and K.X. was performed at the Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. M.J.S. thanks Michael J. Simpson, Jesse W. Wilson, and Francisco E. Robles for sharing their data analysis expertise through helpful discussions and trouble-shooting Python scripts.

Funders	Funder number
Center for Nanophase Materials Sciences
DOE Office of Science
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

big data
dimension reduction
perovskite
photoexcitation
transient absorption microscopy

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10.1021/acsphotonics.5b00638

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title = "Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy",

abstract = "Femtosecond transient absorption microscopy is a novel chemical imaging capability with simultaneous high spatial and temporal resolution. Although several powerful data analysis approaches have been developed and successfully applied to separate distinct chemical species in such images, the application of such analysis to distinguish different photoexcited species is rare. In this paper, we demonstrate a combined approach based on phasor and linear decomposition analysis on a microscopic level that allows us to separate the contributions of both the excitons and free charge carriers in the observed transient absorption response of a composite organometallic lead halide perovskite film. We found spatial regions where the transient absorption response was predominately a result of excitons and others where it was predominately due to charge carriers, and regions consisting of signals from both contributors. Quantitative decomposition of the transient absorption response curves further enabled us to reveal the relative contribution of each photoexcitation to the measured response at spatially resolved locations in the film.",

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AB - Femtosecond transient absorption microscopy is a novel chemical imaging capability with simultaneous high spatial and temporal resolution. Although several powerful data analysis approaches have been developed and successfully applied to separate distinct chemical species in such images, the application of such analysis to distinguish different photoexcited species is rare. In this paper, we demonstrate a combined approach based on phasor and linear decomposition analysis on a microscopic level that allows us to separate the contributions of both the excitons and free charge carriers in the observed transient absorption response of a composite organometallic lead halide perovskite film. We found spatial regions where the transient absorption response was predominately a result of excitons and others where it was predominately due to charge carriers, and regions consisting of signals from both contributors. Quantitative decomposition of the transient absorption response curves further enabled us to reveal the relative contribution of each photoexcitation to the measured response at spatially resolved locations in the film.

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Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy

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Keywords

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