Direct Evidence of Exciton-Exciton Annihilation in Single-Crystalline Organic Metal Halide Nanotube Assemblies

Ying Zhong Ma; Haoran Lin; Mao Hua Du; Benjamin Doughty; Biwu Ma

doi:10.1021/acs.jpclett.8b00761

Direct Evidence of Exciton-Exciton Annihilation in Single-Crystalline Organic Metal Halide Nanotube Assemblies

Ying Zhong Ma, Haoran Lin, Mao Hua Du, Benjamin Doughty, Biwu Ma

Chemical Separations Group

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

18 Scopus citations

Abstract

Excitons in low-dimensional organic-inorganic metal halide hybrid structures are commonly thought to undergo rapid self-trapping following creation due to strong quantum confinement and exciton-phonon interaction. Here we report an experimental study probing the dynamics of these self-trapped excitons in the single-crystalline bulk assemblies of 1D organic metal halide nanotubes, (C₆H₁₃N₄)₃Pb₂Br₇. Through time-resolved photoluminescence (PL) measurements at different excitation intensities, we observed a marked variation in the PL decay behavior that is manifested by an accelerated decay rate with increasing excitation fluence. Our results offer direct evidence of the occurrence of an exciton-exciton annihilation process, a nonlinear relaxation phenomenon that takes place only when some of the self-trapped excitons become mobile and can approach either each other or those trapped excitons. We further identify a fast and dominant PL decay component with a lifetime of ∼2 ns with a nearly invariant relative area for all acquired PL kinetics, suggesting that this rapid relaxation process is intrinsic.

Original language	English
Pages (from-to)	2164-2169
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	9
Issue number	9
DOIs	https://doi.org/10.1021/acs.jpclett.8b00761
State	Published - May 3 2018

Funding

The work at ORNL was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences Geosciences, and Biosciences Division (Y.-Z.M. and B.D.), Materials Sciences and Engineering Division (M.-H.D.). H.L. and B.M. were supported by the Florida State University Energy and Materials Initiative and National Science Foundation (CHE 1664661 and DMR-1709116). The work at ORNL was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division (Y.-Z.M. and B.D.), Materials Sciences and Engineering Division (M.-H.D.). H.L. and B.M. were supported by the Florida State University Energy and Materials Initiative and National Science Foundation (CHE 1664661 and DMR-1709116).

Funders	Funder number
Florida State University Energy and Materials Initiative and National Science Foundation	CHE 1664661
National Science Foundation	1664661, 1709116
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Chemical Sciences, Geosciences, and Biosciences Division
National Science Foundation	DMR-1709116

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10.1021/acs.jpclett.8b00761

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title = "Direct Evidence of Exciton-Exciton Annihilation in Single-Crystalline Organic Metal Halide Nanotube Assemblies",

abstract = "Excitons in low-dimensional organic-inorganic metal halide hybrid structures are commonly thought to undergo rapid self-trapping following creation due to strong quantum confinement and exciton-phonon interaction. Here we report an experimental study probing the dynamics of these self-trapped excitons in the single-crystalline bulk assemblies of 1D organic metal halide nanotubes, (C6H13N4)3Pb2Br7. Through time-resolved photoluminescence (PL) measurements at different excitation intensities, we observed a marked variation in the PL decay behavior that is manifested by an accelerated decay rate with increasing excitation fluence. Our results offer direct evidence of the occurrence of an exciton-exciton annihilation process, a nonlinear relaxation phenomenon that takes place only when some of the self-trapped excitons become mobile and can approach either each other or those trapped excitons. We further identify a fast and dominant PL decay component with a lifetime of ∼2 ns with a nearly invariant relative area for all acquired PL kinetics, suggesting that this rapid relaxation process is intrinsic.",

author = "Ma, {Ying Zhong} and Haoran Lin and Du, {Mao Hua} and Benjamin Doughty and Biwu Ma",

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doi = "10.1021/acs.jpclett.8b00761",

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AU - Ma, Ying Zhong

AU - Lin, Haoran

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AU - Doughty, Benjamin

AU - Ma, Biwu

PY - 2018/5/3

Y1 - 2018/5/3

N2 - Excitons in low-dimensional organic-inorganic metal halide hybrid structures are commonly thought to undergo rapid self-trapping following creation due to strong quantum confinement and exciton-phonon interaction. Here we report an experimental study probing the dynamics of these self-trapped excitons in the single-crystalline bulk assemblies of 1D organic metal halide nanotubes, (C6H13N4)3Pb2Br7. Through time-resolved photoluminescence (PL) measurements at different excitation intensities, we observed a marked variation in the PL decay behavior that is manifested by an accelerated decay rate with increasing excitation fluence. Our results offer direct evidence of the occurrence of an exciton-exciton annihilation process, a nonlinear relaxation phenomenon that takes place only when some of the self-trapped excitons become mobile and can approach either each other or those trapped excitons. We further identify a fast and dominant PL decay component with a lifetime of ∼2 ns with a nearly invariant relative area for all acquired PL kinetics, suggesting that this rapid relaxation process is intrinsic.

AB - Excitons in low-dimensional organic-inorganic metal halide hybrid structures are commonly thought to undergo rapid self-trapping following creation due to strong quantum confinement and exciton-phonon interaction. Here we report an experimental study probing the dynamics of these self-trapped excitons in the single-crystalline bulk assemblies of 1D organic metal halide nanotubes, (C6H13N4)3Pb2Br7. Through time-resolved photoluminescence (PL) measurements at different excitation intensities, we observed a marked variation in the PL decay behavior that is manifested by an accelerated decay rate with increasing excitation fluence. Our results offer direct evidence of the occurrence of an exciton-exciton annihilation process, a nonlinear relaxation phenomenon that takes place only when some of the self-trapped excitons become mobile and can approach either each other or those trapped excitons. We further identify a fast and dominant PL decay component with a lifetime of ∼2 ns with a nearly invariant relative area for all acquired PL kinetics, suggesting that this rapid relaxation process is intrinsic.

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Direct Evidence of Exciton-Exciton Annihilation in Single-Crystalline Organic Metal Halide Nanotube Assemblies

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