Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

doi:10.1007/s11705-020-1931-z

Front. Chem. Sci. Eng.

2021, Vol. 15

Issue (1) : 187-197 https://doi.org/10.1007/s11705-020-1931-z

RESEARCH ARTICLE

Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

Yonghyun Kim¹, Huiwen Liu², Yi Liu², Boa Jin¹, Hao Zhang², Wenjing Tian²(

), Chan Im¹(

)

¹. Department of Chemistry, Konkuk University, Seoul 05029, Korea
². State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China

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Abstract

Cesium lead halide perovskite (CsPbX₃, X= Cl, Br, I) quantum dots (QDs) and their partly Mn²⁺-substituted QDs (CsPb_1–_xMn_xX₃) attract considerable attention owing to their unique photoluminescence (PL) efficiencies. The two types of QDs, having different PL decay dynamics, needed to be further investigated in a form of aggregates to understand their solid-state-induced exciton dynamics in conjunction with their behaviors upon degradation to achieve practical applications of those promising QDs. However, thus far, these QDs have not been sufficiently investigated to obtain deep insights related to the long-term stability of their PL properties as aggregated solid-states. Therefore, in this study, we comparatively examined CsPbX₃- and CsPb_1–_xMn_xX₃-type QDs stocked for>50 d under dark ambient conditions by using excitation wavelength-dependent PL quantum yield and time-resolved PL spectroscopy. These investigations were performed with powder samples in addition to solutions to determine the influence of the inter-QD interaction of the aged QD aggregates on their radiative decays. It turns out that the Mn²⁺-substituted QDs exhibited long-lasting PL quantum efficiencies, while the unsubstituted CsPbX₃-type QDs exhibited a drastic reduction of their PL efficiencies. And the obtained PL traces were clearly sensitive to the sample status. This is discussed with the possible interaction depending on the size and distance of the QD aggregates.

Keywords quantum dots cesium lead halide perovskite time-resolved photoluminescence PL quantum yield QD aggregates

Corresponding Author(s): Wenjing Tian,Chan Im

Online First Date: 28 May 2020 Issue Date: 12 January 2021

Cite this article:

Yonghyun Kim,Huiwen Liu,Yi Liu, et al. Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots[J]. Front. Chem. Sci. Eng., 2021, 15(1): 187-197.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-020-1931-z
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I1/187

Fig.1 Three-dimensional mappings of the combined PL and PLE spectra of (a) DS, (b) CS, and (c) PD of PQD1 and of (d) DS, (e) CS, and (f) PD of PQD2.

Fig.2 Schematics of the (a) DS, (b) CS, and (c) PD QD samples.

Fig.3 UV-vis absorption spectra of (a) a PQD1 dilute solution measured with a two-beam spectrometer, as well as (b) solutions and (c) powders measured with an integrating sphere.

Fig.4 Excitation wavelength-dependent PL spectra of various PQD samples. The legend in (a) also applies to (b) and (c), and that in (f) also applies to (d) and (e).

Tab.1 Steady-state PL results

Fig.5 PL QY spectra of PQD1 and PQD2 samples based on PLE spectra with 20 nm interval between excitation wavelengths.

Fig.6 Time-resolved PL spectra of (a) PQD1-CS and (b) PQD1-PD with excitation wavelength of 350 nm.

Fig.7 Time-resolved slices of the PL band for PQD1-PD shown in Fig. 6(b). A plot of the peak positions in eV scale of the PL slices as a function of time is shown in the inset.

Fig.8 Time-resolved PL decay kinetics of (a) PQD1-DS, (b) PQD1-CS, and (c) PQD1-PD.

Tab.2 Time-resolved PL fitting results

Fig.9 Schematic of the radiative decay paths.

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