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Electron Trapping Prolongs the Lifetime of Charge-Separated States in 2D Perovskite Nanoplatelet-Hole Acceptor Complexes.

ABSTRACT: Two-dimensional (2D) lead halide perovskite nanoplatelets (NPLs) are promising materials for blue light emission because of the strong quantum confinement in the 2D morphology. However, the identity of carrier traps and the trap influence on charge transfer in these NPLs remain unclear. Herein, transient absorption studies revealed two types of electron traps in 3 monolayer lead bromide perovskite NPLs with trapping lifetime of 9.0 ± 0.6 and 516 ± 59 ps, respectively, while no hole traps were observed. Systematic charge transfer experiments show that electron traps have negligible influence on ultrafast electron transfer or hole transfer but extend the half-lifetime of the charge-separated state from 2.1 ± 0.1 to 68 ± 3 ns after hole transfer, which is explained by the reduced electron-hole overlap. This work contributes to the understanding of the fundamental carrier dynamics in 2D perovskite NPLs and offers guidelines for boosting their performance in optoelectronics and photocatalysis.

SUBMITTER: He S

PROVIDER: S-EPMC10009813 | biostudies-literature | 2023 Mar

REPOSITORIES: biostudies-literature

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Electron Trapping Prolongs the Lifetime of Charge-Separated States in 2D Perovskite Nanoplatelet-Hole Acceptor Complexes.

He Sheng S Jin Tao T Ni Anji A Lian Tianquan T

The journal of physical chemistry letters 20230223 9

Two-dimensional (2D) lead halide perovskite nanoplatelets (NPLs) are promising materials for blue light emission because of the strong quantum confinement in the 2D morphology. However, the identity of carrier traps and the trap influence on charge transfer in these NPLs remain unclear. Herein, transient absorption studies revealed two types of electron traps in 3 monolayer lead bromide perovskite NPLs with trapping lifetime of 9.0 ± 0.6 and 516 ± 59 ps, respectively, while no hole traps were ob ...[more]

PMID: 36820889

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Project description:A new set of [Cu(phen)2]+ based rotaxanes, featuring [60]-fullerene as an electron acceptor and a variety of electron donating moieties, namely zinc porphyrin (ZnP), zinc phthalocyanine (ZnPc) and ferrocene (Fc), has been synthesized and fully characterized with respect to electrochemical and photophysical properties. The assembly of the rotaxanes has been achieved using a slight variation of our previously reported synthetic strategy that combines the Cu(i)-catalyzed azide-alkyne cycloaddition reaction (the "click" or CuAAC reaction) with Sauvage's metal-template protocol. To underline our results, complementary model rotaxanes and catenanes have been prepared using the same strategy and their electrochemistry and photo-induced processes have been investigated. Insights into excited state interactions have been afforded from steady state and time resolved emission spectroscopy as well as transient absorption spectroscopy. It has been found that photo-excitation of the present rotaxanes triggers a cascade of multi-step energy and electron transfer events that ultimately leads to remarkably long-lived charge separated states featuring one-electron reduced C60 radical anion (C60?-) and either one-electron oxidized porphyrin (ZnP?+) or one-electron oxidized ferrocene (Fc?+) with lifetimes up to 61 microseconds. In addition, shorter-lived charge separated states involving one-electron oxidized copper complexes ([Cu(phen)2]2+ (? < 100 ns)), one-electron oxidized zinc phthalocyanine (ZnPc?+; ? = 380-560 ns), or ZnP?+ (? = 2.3-8.4 ?s), and C60?- have been identified as intermediates during the sequence. Detailed energy diagrams illustrate the sequence and rate constants of the photophysical events occurring with the mechanically-linked chromophores. This work pioneers the exploration of mechanically-linked systems as platforms to position three distinct chromophores, which are able to absorb light over a very wide range of the visible region, triggering a cascade of short-range energy and electron transfer processes to afford long-lived charge separated states.

Dataset Information

Electron Trapping Prolongs the Lifetime of Charge-Separated States in 2D Perovskite Nanoplatelet-Hole Acceptor Complexes.

Publications

Electron Trapping Prolongs the Lifetime of Charge-Separated States in 2D Perovskite Nanoplatelet-Hole Acceptor Complexes.

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