Material Design and Optoelectronic Properties of Three-Dimensional Quadruple Perovskite Halides

Lin, Yuanzhang; Hu, Shanshan; Xia, Bing; Fan, Kaiqing; Gong, Linghui; Kong, Jintao; Huang, Xiao‐Ying; Xiao, Zewen; Du, Ke‐Zhao

doi:10.1021/acs.jpclett.9b01757

Cited by 74 publications

(95 citation statements)

References 55 publications

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“…The PXRD results were also compared with results from the calculation based on the trigonal R3̅ m structure ( Figure S1, Supporting Information). The PXRD patterns of the four types of NCs are consistent with the calculation and the bulk samples, [21][22][23][24] which confirm the formation of a pure quadruple-perovskite phase.…”

supporting

confidence: 80%

“…[ 13 ] The normalized absorption spectra and the corresponding bandgaps of these four NCs are shown in Figure S5 (Supporting Information). The bandgap of quadruple‐perovskite NCs are slightly larger than the bulk samples, [ 21–24 ] which indicate the small quantum confinement effect. Next, the PL properties of these NCs are studied.…”

Section: Figurementioning

confidence: 99%

“…Rietveld refinements of the PXRD patterns indicated a trigonal R3̅ m space group for all four types of NCs, which correspond to a vacancy-ordered quadruple-perovskite structure. [21][22][23][24] The structural parameters, which were extracted from the refinements of these NCs, are given in Tables S1-S5 (Supporting Information). Typically, the vacancy-ordered structure of Cs 4 CdSb 2 Cl 12 results in a triple-layered (n = 3) perovskite with alternating corners, sharing CdCl 6 and SbCl 6 octahedra.…”

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confidence: 99%

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Efficient Luminescent Halide Quadruple‐Perovskite Nanocrystals via Trap‐Engineering for Highly Sensitive Photodetectors

et al. 2021

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elements to replace lead due to the high toxicity. Lead-free halide perovskite NCs have recently received increasing attention for their low toxicity, high stability, and chemical diversity. [3-8] The most direct way is usually isovalent substitution of Pb 2+ with Sn 2+. [3] Unfortunately, lead-free CsSnX 3 (X = Cl, Br, and I) NCs is extremely unstable because of the easy oxidation of Sn 2+ into Sn 4+ in air. [3] Subsequently, A 3 M ' 2 X 9-type layer perovskite, A 2 MM ' X 6-type, and A 2 BX 6-type double perovskite (where A denotes alkali-metal ions; M, M' and B denotes monovalent-, trivalent-, and tetravalent-cations; X denotes halogen ions) with high stability have been reported. [9-20] However, optoelectronic devices based on these lead-free perovskite NCs have made limited progress. Such as, photodetectors based on lead-free perovskite NCs exhibited low responsivity (typically <1 A W −1). [17,18] This is mainly due to the low crystallinity, prominent charge-carrier trapping, and short charge-carrier lifetimes of these NCs. In this paper, we report, for the first time, the colloidal synthesis of a series of trigonal (R3̅ m) vacancy-ordered quadrupleperovskite NCs, i.e., Cs 4 CdSb 2 Cl 12 , Cs 4 MnSb 2 Cl 12 , Cs 4 CdBi 2 Cl 12 , and Cs 4 MnBi 2 Cl 12. The photoluminescence quantum yield (PLQY) can be enhanced by 96-fold while the PL lifetime can be enhanced by 77-fold in Cs 4 MnBi 2 Cl 12 NCs through metal alloying. Studies of the charge-carrier dynamics including temperature-dependent PL and femtosecond (fs) transient absorption (TA) measurements were performed to clarify the mechanism of the PL enhancement, which is due to the elimination of the charge-carrier trapping process and increased crystallinity. Besides, the PL-peak position can be tuned continuously from 590 to 640 nm by changing the MnCl bond distance via metal alloying. Finally, we fabricate photodetectors based on quadruple-perovskite NCs, which exhibit high responsivity (0.98 × 10 4 A W −1) and an EQE of 3 × 10 6 %. The responsivity is much higher than previous reported photodetectors base on lead-free perovskite NCs. These results show that quadruple-perovskite NCs open new possibilities for optoelectronic applications. The colloidal synthesis of halide quadruple-perovskite NCs was performed using a modified hot-injection method-for details see the Experimental Section. [14] As shown in Figure 1a,b, replacing M in A 2 MM'X 6 with one M'' (M'' denotes a +2 cation) The colloidal synthesis of a new type of lead-free halide quadruple-perovskite nanocrystals (NCs) is reported. The photoluminescence quantum yield and charge-carrier lifetime of quadruple-perovskite NCs can be enhanced by 96 and 77-fold, respectively, via metal alloying. Study of charge-carrier dynamics provide solid demonstrate that the PL enhancement is due to the elimination of ultrafast (1.4 ps) charge-carrier trapping processes in the alloyed NCs. Thanks to the high crystallinity, low trap-state density, and long carrier lifetime (193.4 μs), the alloyed quadruple-perovskite N...

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confidence: 80%

Section: Figurementioning

confidence: 99%

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confidence: 99%

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Efficient Luminescent Halide Quadruple‐Perovskite Nanocrystals via Trap‐Engineering for Highly Sensitive Photodetectors

et al. 2021

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“…Vacancy‐ordered layered HDPs are suitable hosts for bivalent substitution, which covers the shortage for limited bivalent doping in HDPs, such as Cu 2+ , Mn 2+ , and Cd 2+ . [ 119,125–127 ] Recently, Cai et al synthesized Cs 4 Cu x Ag 2−2 x Sb 2 Cl 12 (0 ≤ x ≤ 1) NCs with a uniform sphere‐like shape for the first time. [ 123 ] The vacancy‐ordered HDP NCs have electronic band structural transition from a wide indirect bandgap to a narrow direct bandgap with increased Cu content.…”

Section: Structural Diversity Of Hdpsmentioning

confidence: 99%

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Zeng

2020

Small Structures

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Organic–inorganic halide perovskites have attracted extensive attention due to their excellent optoelectronic properties. However, the toxicity of heavy atom Pb2+ and instability overshadow further commercial applications, motivating researchers to explore alternative analogues to overcome these disadvantages. Lead‐free halide double perovskites (HDPs), sharing similar crystal structures with organic–inorganic halide perovskites, are promising candidates for optoelectronic applications. However, HDPs possess unique properties that are uncommon in organic–inorganic halide perovskites deriving from feasible component engineering and strong electron–phonon interaction. Bright luminescence in HDPs originates from self‐trapped excitons (STEs) and sensitized dopants can cover the full visible and near‐infrared ray (NIR) gamut by modulating parity‐forbidden transitions and the energy‐transfer process. The superior optoelectronic characteristics of HDPs further extend applications on self‐assembly, white‐light phosphors, NIR bioimaging, and scintillators, in comparison to organic–inorganic halide perovskites. Herein, the structural diversity, tunable luminescence, photophysical mechanism of STEs, charge‐carrier dynamics, size effect, and stability issues of HDPs are discussed. The challenges and outlook for further investigations are also given, which may help in discovering new analogues and boosting the photoluminescence quantum yield and stability of HDPs.

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“…, 2B IV → B III + B V ). [ 52 ] Though the applications of halide perovskites have been widely explored, the elementary halogen storage has rarely been studied therein. As a kind of halogen‐rich materials, the halide perovskites could be developed for halogen chemisorption if the halide anions could be converted into elementary halogens.…”

Section: Introductionmentioning

confidence: 99%

Reversible Release and Fixation of Bromine in Vacancy‐Ordered Bromide Perovskites

Lin

Xia

et al. 2020

Energy & Environ Materials

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Material Design and Optoelectronic Properties of Three-Dimensional Quadruple Perovskite Halides

Cited by 74 publications

References 55 publications

Efficient Luminescent Halide Quadruple‐Perovskite Nanocrystals via Trap‐Engineering for Highly Sensitive Photodetectors

Efficient Luminescent Halide Quadruple‐Perovskite Nanocrystals via Trap‐Engineering for Highly Sensitive Photodetectors

Lead‐Free Halide Double Perovskites: Structure, Luminescence, and Applications

Reversible Release and Fixation of Bromine in Vacancy‐Ordered Bromide Perovskites

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