Morphology-Independent Stable White-Light Emission from Self-Assembled Two-Dimensional Perovskites Driven by Strong Exciton–Phonon Coupling to the Organic Framework

Thirumal, Krishnamoorthy; Chong, Wee Kiang; Xie, Wei; Ganguly, Rakesh; Muduli, Subas; Sherburne, Matthew; Asta, Mark; Mhaisalkar, Subodh; Sum, Tze Chien; Soo, Han Sen; Mathews, Nripan

doi:10.1021/acs.chemmater.7b00073

Cited by 206 publications

(211 citation statements)

References 34 publications

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“…Furthermore,t he corresponding correlated color temperatures (CCT) can be tuned from 7034 Kt o 4188 K ( Figure 2c), and the photoluminescence quantum yield (PLQY) can reach 68 %( Supporting Information, Table S3). Among these samples,T PbBr-3 (Mn content of 0.027 %) is particularly interesting.I ts CRI reaches 96 corresponding to the record CRI for as ingle phase emitter, [25,41,42] the CIE coordinate (0.330, 0.365) corresponds to pure white light, and the PLQY reaches 60 %which is anew record for lead halide white emitter (Figure 2c< xfigr2). [17,20-22, 25, 43] Even if other compounds such as (H 2 DABCO)(Pb 2 Cl 6 )a nd (C 5 H 7 N 2 ) 2 SnBr 4 were reported…”

Section: Resultsmentioning

confidence: 95%

“…70-90) owing to the broadband emission. [16,23,25] However,i ns ome color-critical high-level applications,s uch as jewelry,photography,museums,and surgery,anultra-high CRI is required. [26] Through the comparison of the resulting emissions with solar spectrum (Supporting Information, Figure S1), it is observed that such emitters are not satisfactory for these applications,b ecause of the lack of either blue or/ and red components.T hus,a dding an appropriate emission band through doping can be an interesting strategy to improve the color rendering of such light sources.…”

Section: Introductionmentioning

confidence: 99%

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Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

et al. 2020

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Near-UV-pumped white-light-emitting diodes with ultra-high color rendering and decreased blue-light emission is highly desirable.H owever,d iscovering as ingle-phase white light emitter with such characteristics remains challenging. Herein, we demonstrate that Mn doping as lowa s0 .027 %i n the hybrid post-perovskite type (TDMP)PbBr 4 (TDMP = trans-2,5-dimethylpiperaziniium) enables to achieve ab right pure white emission replicating the spectrum of the sunsrays. Thus,awhite phosphor exhibiting an emission with CIE coordinates (0.330, 0.365), ahigh photoluminescence quantum yield of 60 %( new recordf or white light emission of hybrid lead halides), and an ultra-high color rendering index (CRI = 96, R9 = 91.8), corresponding to the recordv alue for as ingle phase emitter was obtained. The investigation of the photoluminescence properties revealed how free excitons,s elftrapped excitons,and lowamount of Mn dopants are coupled to give rise to such pure white emission.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

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Section: Resultsmentioning

confidence: 95%

Section: Introductionmentioning

confidence: 99%

Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

et al. 2020

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“…[6] The stable self-trapped excitons in a deformable lattice can result in a highly distorted excited state with respect to the ground state. [7] On the contrary, (PEA) 2 PbBr 4 with relatively smaller distorted lattice only exhibits narrow free exciton emission. At ambient conditions, the broadband emission of (PEA) 2 PbCl 4 was observed to originate from self-trapped excitons in a highly distorted structure.…”

Section: Doi: 101002/advs201801628mentioning

confidence: 98%

Pressure‐Induced Broadband Emission of 2D Organic–Inorganic Hybrid Perovskite (C₆H₅C₂H₄NH₃)₂PbBr₄

Zhang

Wang

et al. 2018

Advanced Science

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Abstract2D Ruddlesden–Popper halide perovskites, which incorporate hydrophobic organic interlayers to considerably improve environmental stability and optical properties diversity, have attracted substantial research attention for optoelectronic applications. The burgeoning broad emission arising from exciton self‐trapping of 2D perovskites shows a strong dependence on a deformable structure. Here, the pressure‐induced broadband emission of layered (001) Pb‐Br perovskite with a large Stokes shift in the visible region is observed by finely improving lattice distortion to increase exciton–phonon coupling under hydrostatic pressure. Band gap narrows ≈0.5 eV under modest pressure, mainly due to the large compressibility of the orientational organic layer, confirming that the bulky organic cations notably influence the structure and, in turn, the various properties of materials. Sequential amorphization of the organic and inorganic layer is confirmed by high pressure Raman and X‐ray diffraction measurements, suggesting the particularity of layered crystal structures. The mechanism constructed here offers a new route for tuning the optical properties of 2D perovskites.

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“…With decreasing temperature, the RPP PL peaks generally become narrower and more symmetric. The broadened asymmetric PL shape at room temperature typically arises because of phonon scattering and self‐trapped excitons (low photon energy emission) . At low injected carrier density, this broadening is believed to primarily arise from exciton–phonon interactions .…”

Section: Auger Decay Lifetime (τAuger) At High Excitation Fluence (P mentioning

confidence: 99%

Lasing from Mechanically Exfoliated 2D Homologous Ruddlesden–Popper Perovskite Engineered by Inorganic Layer Thickness

et al. 2019

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approach to realize new functionalities through facile van der Waals coupled 2D layers. [6] Owing to the large dielectric mismatch between the inorganic and organic layers, the quasi-2D RPPs naturally form quantum well structures, in which, the inorganic and organic layers serve as potential wells and barriers, respectively. [7] Moreover, these quantum confined structures impart the appealing characteristics of improved environmental stability and enhanced exciton confinement. [2] These make the quasi-2D RPPs promising for solar cell and light-emitting diode (LED) applications. [5,[8][9][10] Recently, the amplified spontaneous emission (ASE) and lasing behaviors of 2D RPPs have been demonstrated. [11][12][13][14][15][16][17] However, the lasing is mostly obtained from solution-processed spin-coated thin films, in which multiple RPP components inevitably form with different bandgaps that drive cascade carrier transfer and may reshape the build-up of population inversion. [11,14,15,18] Also, the development of continuous-wave or electrically driven RPP lasers central for practical applications is still challenging. The exploitation of homologous RPP lasers is of great importance to gain further insights into the intrinsic lasing mechanisms of these quantum well-like structures as well as the design of low-threshold 2D 2D Ruddlesden-Popper perovskites (RPPs) have aroused growing attention in light harvesting and emission applications owing to their high environmental stability. Recently, coherent light emission of RPPs was reported, however mostly from inhomologous thin films that involve cascade intercompositional energy transfer. Lasing and fundamental understanding of intrinsic laser dynamics in homologous RPPs free from intercompositional energy transfer is still inadequate. Herein, the lasing and loss mechanisms of homologous 2D (BA) 2 (MA) n −1 Pb n I 3n+1 RPP thin flakes mechanically exfoliated from the bulk crystal are reported. Multicolor lasing is achieved from the large-n RPPs (n ≥ 3) in the spectral range of 620-680 nm but not from small-n RPPs (n ≤ 2) even down to 78 K. With decreasing n, the lasing threshold increases significantly and the characteristic temperature decreases as 49, 25, and 20 K for n = 5, 4, and 3, respectively. The n-engineered lasing behaviors are attributed to the stronger Auger recombination and exciton-phonon interaction as a result of the enhanced quantum confinement in the smaller-n perovskites. These results not only advance the fundamental understanding of loss mechanisms in both inhomologous and homologous RPP lasers but also provide insights into developing low-threshold, substrate-free, and multicolor 2D semiconductor microlasers.2D Ruddlesden-Popper perovskites (RPPs), with the general chemical formula of L 2 (MA) n−1 M n X 3n+1 , are composed of welldefined inorganic layers with corner connected [MX 6 ] 4− octahedra and long organic chains (L + ) intercalated between these inorganic fragments. [1][2][3][4][5] This structure promises a viable

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Morphology-Independent Stable White-Light Emission from Self-Assembled Two-Dimensional Perovskites Driven by Strong Exciton–Phonon Coupling to the Organic Framework

Cited by 206 publications

References 34 publications

Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

Pressure‐Induced Broadband Emission of 2D Organic–Inorganic Hybrid Perovskite (C₆H₅C₂H₄NH₃)₂PbBr₄

Lasing from Mechanically Exfoliated 2D Homologous Ruddlesden–Popper Perovskite Engineered by Inorganic Layer Thickness

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Morphology-Independent Stable White-Light Emission from Self-Assembled Two-Dimensional Perovskites Driven by Strong Exciton–Phonon Coupling to the Organic Framework

Cited by 206 publications

References 34 publications

Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

Doped Lead Halide White Phosphors for Very High Efficiency and Ultra‐High Color Rendering

Pressure‐Induced Broadband Emission of 2D Organic–Inorganic Hybrid Perovskite (C6H5C2H4NH3)2PbBr4

Lasing from Mechanically Exfoliated 2D Homologous Ruddlesden–Popper Perovskite Engineered by Inorganic Layer Thickness

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Pressure‐Induced Broadband Emission of 2D Organic–Inorganic Hybrid Perovskite (C₆H₅C₂H₄NH₃)₂PbBr₄