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Title: Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations

Abstract

Here, photo-generated charge carrier dynamics in Ruddlesden–Popper 2D perovskites with linear (n-BA) and branched (iso-BA) butylamine as spacing cations have been studied by using transient absorption and time-resolved photoluminescence spectroscopies. Both n-BA and iso-BA perovskites consist of mixed-phase 2D quantum wells with various layer thicknesses, where the photo-generated charges undergo inter-phase charge transfer from thinner quantum wells to thicker ones. By shortening the spacer from n-BA to iso-BA, the transfer rates are significantly increased, which can also diminish the charge accumulation in thin quantum wells induced by the unbalanced electron and hole charge transfer rates. Under high excitation intensity, the shorter spacing cation is found to further facilitate the energy transfer, which can compete with fast high-order carrier recombination and consequently improve the charge transfer efficiency. Intriguingly, we observe the existence of extra bulk 3D phases embedded within iso-BA perovskites, which can efficiently collect the confined charges within 2D phases and then transport them with faster carrier mobility and slower recombination rates.

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [3];  [4];  [5];  [6]; ORCiD logo [2];  [3]
  1. Lund Univ., Lund (Sweden); Qatar Univ., Doha (Qatar)
  2. Fudan Univ., Shanghai (China)
  3. Lund Univ., Lund (Sweden)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. ELI-ALPS, ELI-HU Non-Profit Ltd., Szeged (Hungary); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Qatar National Research Fund (QNRF); Swedish Research Council (SRC); European Regional Development Fund (ERDF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1489254
Alternate Identifier(s):
OSTI ID: 1434137
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 15; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zheng, Kaibo, Chen, Yani, Sun, Yong, Chen, Junsheng, Chábera, Pavel, Schaller, Richard, Al-Marri, Mohammed J., Canton, Sophie E., Liang, Ziqi, and Pullerits, Tõnu. Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations. United States: N. p., 2018. Web. doi:10.1039/c8ta01518j.
Zheng, Kaibo, Chen, Yani, Sun, Yong, Chen, Junsheng, Chábera, Pavel, Schaller, Richard, Al-Marri, Mohammed J., Canton, Sophie E., Liang, Ziqi, & Pullerits, Tõnu. Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations. United States. doi:10.1039/c8ta01518j.
Zheng, Kaibo, Chen, Yani, Sun, Yong, Chen, Junsheng, Chábera, Pavel, Schaller, Richard, Al-Marri, Mohammed J., Canton, Sophie E., Liang, Ziqi, and Pullerits, Tõnu. Fri . "Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations". United States. doi:10.1039/c8ta01518j. https://www.osti.gov/servlets/purl/1489254.
@article{osti_1489254,
title = {Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations},
author = {Zheng, Kaibo and Chen, Yani and Sun, Yong and Chen, Junsheng and Chábera, Pavel and Schaller, Richard and Al-Marri, Mohammed J. and Canton, Sophie E. and Liang, Ziqi and Pullerits, Tõnu},
abstractNote = {Here, photo-generated charge carrier dynamics in Ruddlesden–Popper 2D perovskites with linear (n-BA) and branched (iso-BA) butylamine as spacing cations have been studied by using transient absorption and time-resolved photoluminescence spectroscopies. Both n-BA and iso-BA perovskites consist of mixed-phase 2D quantum wells with various layer thicknesses, where the photo-generated charges undergo inter-phase charge transfer from thinner quantum wells to thicker ones. By shortening the spacer from n-BA to iso-BA, the transfer rates are significantly increased, which can also diminish the charge accumulation in thin quantum wells induced by the unbalanced electron and hole charge transfer rates. Under high excitation intensity, the shorter spacing cation is found to further facilitate the energy transfer, which can compete with fast high-order carrier recombination and consequently improve the charge transfer efficiency. Intriguingly, we observe the existence of extra bulk 3D phases embedded within iso-BA perovskites, which can efficiently collect the confined charges within 2D phases and then transport them with faster carrier mobility and slower recombination rates.},
doi = {10.1039/c8ta01518j},
journal = {Journal of Materials Chemistry. A},
number = 15,
volume = 6,
place = {United States},
year = {2018},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 9 works
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Figures / Tables:

Figure 1 Figure 1: (a) XRD patterns of n-BA and iso-BA perovskite film with corresponding chemical and crystal structures. (b) UV-vis absorption (solid lines) and PL (dashed lines) spectra of as-obtained n-BA and iso-BA perovskite films, in which the characteristic exciton bands for 2D quantum wells with different thicknesses are indicated.

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    Works referencing / citing this record:

    Strong thickness-dependent quantum confinement in all-inorganic perovskite Cs 2 PbI 4 with a Ruddlesden–Popper structure
    journal, January 2019

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