Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.

Navendu Mondal; Rounak Naphade; Xiaohe Zhou; Yangzi Zheng; Kwangjae Lee; Issam Gereige; Ahmed Al-Saggaf; Osman Bakr; Omar F. Mohammed; Yuri N. Gartstein; Anton V. Malko

doi:10.1021/acs.jpclett.9b03709

Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.

Navendu Mondal, Rounak Naphade, Xiaohe Zhou, Yangzi Zheng, Kwangjae Lee, Issam Gereige, Ahmed Al-Saggaf, Osman Bakr, Omar F. Mohammed, Yuri N. Gartstein, Anton V. Malko

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Abstract

Time-resolved photoluminescence (PL) and femtosecond transient absorption (TA) spectroscopy are employed to study the photoexcitation dynamics in a highly emissive two-dimensional perovskite compound (en)4Pb2Br9·3Br with the ethylene diammonium (en) spacer. We find that while the PL kinetics is substantially T-dependent over the whole range of studied temperatures T ∼ 77-350 K, the PL quantum yield remains remarkably nearly T-independent up to T ∼ 280-290 K, appreciably decreasing only at higher temperatures. Considerable differences are also revealed between the TA spectra and the responses to the excitation power at low and at room temperatures. Numerical solutions of Onsager-Braun-type kinetic-diffusion equations illustrate that the salient features of the experimental observations are consistent with the picture of a T-dependent dynamic interplay between tightly bound emissive excitons and larger-size, loosely bound, nonemissive geminate charge pairs arising already at earlier relaxation times. The geminate pairs play the role of

Original language	English (US)
Pages (from-to)	1112-1119
Number of pages	8
Journal	The Journal of Physical Chemistry Letters
Volume	11
Issue number	3
DOIs	https://doi.org/10.1021/acs.jpclett.9b03709
State	Published - Jan 27 2020

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https://repository.kaust.edu.sa/bitstream/10754/661347/1/jz-2019-03709b_Submitted%20ver.pdf

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Mondal, N., Naphade, R., Zhou, X., Zheng, Y., Lee, K., Gereige, I., Al-Saggaf, A., Bakr, O., Mohammed, O. F., Gartstein, Y. N., & Malko, A. V. (2020). Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model. The Journal of Physical Chemistry Letters, 11(3), 1112-1119. https://doi.org/10.1021/acs.jpclett.9b03709

@article{32531a1cd34543ea8a0a4c5eb55b8713,

title = "Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.",

abstract = "Time-resolved photoluminescence (PL) and femtosecond transient absorption (TA) spectroscopy are employed to study the photoexcitation dynamics in a highly emissive two-dimensional perovskite compound (en)4Pb2Br9·3Br with the ethylene diammonium (en) spacer. We find that while the PL kinetics is substantially T-dependent over the whole range of studied temperatures T ∼ 77-350 K, the PL quantum yield remains remarkably nearly T-independent up to T ∼ 280-290 K, appreciably decreasing only at higher temperatures. Considerable differences are also revealed between the TA spectra and the responses to the excitation power at low and at room temperatures. Numerical solutions of Onsager-Braun-type kinetic-diffusion equations illustrate that the salient features of the experimental observations are consistent with the picture of a T-dependent dynamic interplay between tightly bound emissive excitons and larger-size, loosely bound, nonemissive geminate charge pairs arising already at earlier relaxation times. The geminate pairs play the role of",

author = "Navendu Mondal and Rounak Naphade and Xiaohe Zhou and Yangzi Zheng and Kwangjae Lee and Issam Gereige and Ahmed Al-Saggaf and Osman Bakr and Mohammed, {Omar F.} and Gartstein, {Yuri N.} and Malko, {Anton V.}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: The work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0010697.",

year = "2020",

month = jan,

day = "27",

doi = "10.1021/acs.jpclett.9b03709",

language = "English (US)",

volume = "11",

pages = "1112--1119",

journal = "The Journal of Physical Chemistry Letters",

issn = "1948-7185",

publisher = "American Chemical Society",

number = "3",

}

Mondal, N, Naphade, R, Zhou, X, Zheng, Y, Lee, K, Gereige, I, Al-Saggaf, A, Bakr, O , Mohammed, OF, Gartstein, YN & Malko, AV 2020, 'Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.', The Journal of Physical Chemistry Letters, vol. 11, no. 3, pp. 1112-1119. https://doi.org/10.1021/acs.jpclett.9b03709

TY - JOUR

T1 - Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.

AU - Mondal, Navendu

AU - Naphade, Rounak

AU - Zhou, Xiaohe

AU - Zheng, Yangzi

AU - Lee, Kwangjae

AU - Gereige, Issam

AU - Al-Saggaf, Ahmed

AU - Bakr, Osman

AU - Mohammed, Omar F.

AU - Gartstein, Yuri N.

AU - Malko, Anton V.

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: The work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0010697.

PY - 2020/1/27

Y1 - 2020/1/27

N2 - Time-resolved photoluminescence (PL) and femtosecond transient absorption (TA) spectroscopy are employed to study the photoexcitation dynamics in a highly emissive two-dimensional perovskite compound (en)4Pb2Br9·3Br with the ethylene diammonium (en) spacer. We find that while the PL kinetics is substantially T-dependent over the whole range of studied temperatures T ∼ 77-350 K, the PL quantum yield remains remarkably nearly T-independent up to T ∼ 280-290 K, appreciably decreasing only at higher temperatures. Considerable differences are also revealed between the TA spectra and the responses to the excitation power at low and at room temperatures. Numerical solutions of Onsager-Braun-type kinetic-diffusion equations illustrate that the salient features of the experimental observations are consistent with the picture of a T-dependent dynamic interplay between tightly bound emissive excitons and larger-size, loosely bound, nonemissive geminate charge pairs arising already at earlier relaxation times. The geminate pairs play the role of

AB - Time-resolved photoluminescence (PL) and femtosecond transient absorption (TA) spectroscopy are employed to study the photoexcitation dynamics in a highly emissive two-dimensional perovskite compound (en)4Pb2Br9·3Br with the ethylene diammonium (en) spacer. We find that while the PL kinetics is substantially T-dependent over the whole range of studied temperatures T ∼ 77-350 K, the PL quantum yield remains remarkably nearly T-independent up to T ∼ 280-290 K, appreciably decreasing only at higher temperatures. Considerable differences are also revealed between the TA spectra and the responses to the excitation power at low and at room temperatures. Numerical solutions of Onsager-Braun-type kinetic-diffusion equations illustrate that the salient features of the experimental observations are consistent with the picture of a T-dependent dynamic interplay between tightly bound emissive excitons and larger-size, loosely bound, nonemissive geminate charge pairs arising already at earlier relaxation times. The geminate pairs play the role of

UR - http://hdl.handle.net/10754/661347

UR - https://pubs.acs.org/doi/10.1021/acs.jpclett.9b03709

UR - http://www.scopus.com/inward/record.url?scp=85079076325&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.9b03709

DO - 10.1021/acs.jpclett.9b03709

M3 - Article

C2 - 31958009

SN - 1948-7185

VL - 11

SP - 1112

EP - 1119

JO - The Journal of Physical Chemistry Letters

JF - The Journal of Physical Chemistry Letters

IS - 3

ER -

Dynamical Interconversion between Excitons and Geminate Charge Pairs in Two-Dimensional Perovskite Layers Described by the Onsager-Braun Model.

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