Structural origins of broadband emission from layered Pb–Br hybrid perovskites

Smith, Matthew D.; Jaffe, Adam B.; Dohner, Emma R.; Lindenberg, Aaron M.; Karunadasa, Hemamala I.

doi:10.1039/c7sc01590a

Cited by 483 publications

(763 citation statements)

References 54 publications

Supporting

Mentioning

710

Contrasting

Order By: Relevance

“…Mater. [1,25] Therefore, the linear dependence of PL intensity on the excitation power indicates that the white-light emission of CsCu 2 I 3 SC does not originate from the permanent defects. The key parameters of white-light perovskites are summarized in Table 2.…”

Section: T Imentioning

confidence: 96%

“…[21][22][23] Similarly, we attribute the broadband luminescence of CsCu 2 I 3 to self-trapped excitons recombination, in whose mechanism the distortion of lattice is the main cause of Stokes shift. [2,25] In the X 2 exciton, the emission peaks show a slight blueshift with increasing temperature. In our work, the emission of CsCu 2 I 3 has a highly Stokes shift of 1.51 eV, which demonstrates the self-trapped exciton recombination.…”

Section: Doi: 101002/adma201905079mentioning

confidence: 99%

See 1 more Smart Citation

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

et al. 2019

View full text Add to dashboard Cite

In order to achieve a high quantum efficiency, doping crystals with appropriate elements such as sodium cations (ref. [8]) to reduce electronic dimension is a useful method. [5,8] However, doping also tends to cause nonradiation recombination loss. [13] Therefore, a reliable and promising way is to synthesize high-quality inorganic metal halide single crystal (SC) with natural lowdimensional structure to realize stable and high quantum efficiency white-light illumination application.In this work, we successfully synthesized 1D CsCu 2 I 3 SC by replacing toxic Pb with eco-friendly and abundant Cu, and organic molecules with large-radius Cs. [12,13] The "one dimension" we noted here is localized dimension of electron. [14] Through density functional theory (DFT) calculation, in 1D CsCu 2 I 3 SC, [Cu 2 I 3 ] − octahedra contributes most electronic states, and Cs + only forms a 1D electronic structure with isolated [Cu 2 I 3 ] − in 2D direction. Therefore, CsCu 2 I 3 SC obtains a high photoluminescence quantum yield (PLQY ≈15.7%) of the IWE at room temperature. [2] We also calculated that the crystal has a high radiation recombination rate which is owning to the 1D localized electronic structure, and this rate is the key to its high PLQY. [15,16] Under a strong injection and atmospheric environment, the PL intensity of all-inorganic CsCu 2 I 3 SC only decays about 5% after 750 min ( Figure S5, Supporting Information). This excellent stability demonstrates that the all-inorganic CsCu 2 I 3 SC possesses a great prospect in high-efficiency lighting applications.High-quality CsCu 2 I 3 SCs were synthesized by antisolvent infiltration method. [17,18] Cesium iodide and cuprous (I) iodide in certain ratio were dissolved in dimethyl formamide (DMF)dimethyl sulfoxide (DMSO) (4:1) to obtain a saturated solution. Then, methanol (antisolvent) was slowly dropped into the saturated solution to form a white precipitate (the white precipitate quickly dissolved again) until it no longer dissolved. The solution was filtered and then placed in a beaker with methanol atmosphere to grow crystals. Several days later, centimeter-scale high-quality CsCu 2 I 3 SCs were obtained (refer to the Supporting information and the Experimental Section for more details). Figure 1a shows an optical image of a rod-shaped CsCu 2 I 3 SCs excited by ultraviolet light. The SC has a size of about 10 mm × 1.5 mm, being colorless and transparent at room temperature but having strong white-light emission under ultraviolet light. Crystal structure of the CsCu 2 I 3 SC was obtained through single-crystal X-ray diffraction (SCXRD) test (Figure 1b,c), which belongs to orthorhombic system. The 1D Energy-saving white lighting from the efficient intrinsic emission of semiconductors is considered as a next-generation lighting source. Currently, white-light emission can be composited with a blue light-emitting diode and yellow phosphor. However, this solution has an inevitable light loss, which makes the improvement of the energy utilization efficiency more difficult. T...

show abstract

Section: T Imentioning

confidence: 96%

Section: Doi: 101002/adma201905079mentioning

confidence: 99%

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

et al. 2019

View full text Add to dashboard Cite

show abstract

“…This finding agrees well with the earlier study by Karunadasa et al that only the out-of-plane Pb-(m-Br)-Pb angle (among at otal of 52 structural parameters) is closely correlated with the intensity of broadband emission. [37] Thez igzag chain is substantially flattened, with an increase in the Pb-(m 2 )Br-Pb bond from 128.4888 8 to 146.8928 8 (Figure 3c). Thel arge distortion (D tilt )a ngle of % 51.58 8 is larger than that of many white-light-emitting perovskites in the previous study.…”

Section: Angewandte Chemiementioning

confidence: 99%

Intrinsic White‐Light‐Emitting Metal–Organic Frameworks with Structurally Deformable Secondary Building Units

et al. 2019

View full text Add to dashboard Cite

show abstract

“…11,18,21,90 If the green PL were to originate from a midgap state or a trap state, then the absorption of the Cs 4 PbBr 6 host would remain unaltered, i.e., it would have no features in the visible range. Take, for example, the case of fluorescent, low-dimensional organic–inorganic lead or tin halides, 85,91−94 in which the dimensionality (whether 2D, 1D, or 0D) is tuned by using specially designed amines, like 2,2′-(ethylenedioxy)bis(ethylamine), C 4 N 2 H 14 2+ , or C 4 N 2 H 14 Br + . In all of these low-dimensional organic lead and tin halides, the strong dimensional confinement results in large bandgaps in the ultraviolet region of the spectrum, and powders of all of these materials are, indeed, white in color.…”

mentioning

confidence: 99%

Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges

Akkerman

Abdelhady

Manna

2018

J. Phys. Chem. Lett.

236

247

View full text Add to dashboard Cite

Over the past decade, lead halide perovskites (LHPs) have emerged as new promising materials in the fields of photovoltaics and light emission due to their facile syntheses and exciting optical properties. The enthusiasm generated by LHPs has inspired research in perovskite-related materials, including the so-called “zero-dimensional cesium lead halides”, which will be the focus of this Perspective. The structure of these materials is formed of disconnected lead halide octahedra that are stabilized by cesium ions. Their optical properties are dominated by optical transitions that are localized within the individual octahedra, hence the title “‘zero-dimensional perovskites”. Controversial results on their physical properties have recently been reported, and the true nature of their photoluminescence is still unclear. In this Perspective, we will take a close look at these materials, both as nanocrystals and as bulk crystals/thin films, discuss the contrasting opinions on their properties, propose potential applications, and provide an outlook on future experiments.

show abstract

Structural origins of broadband emission from layered Pb–Br hybrid perovskites

Abstract: We present synthetic design rules for achieving and optimizing broadband emission from layered halide perovskites.

Cited by 483 publications

References 54 publications

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

Intrinsic White‐Light‐Emitting Metal–Organic Frameworks with Structurally Deformable Secondary Building Units

Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges

Contact Info

Product

Resources

About

Structural origins of broadband emission from layered Pb–Br hybrid perovskites

Abstract: We present synthetic design rules for achieving and optimizing broadband emission from layered halide perovskites.

Cited by 483 publications

References 54 publications

All‐Inorganic CsCu2I3 Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

All‐Inorganic CsCu2I3 Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

Intrinsic White‐Light‐Emitting Metal–Organic Frameworks with Structurally Deformable Secondary Building Units

Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges

Contact Info

Product

Resources

About

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination

All‐Inorganic CsCu₂I₃ Single Crystal with High‐PLQY (≈15.7%) Intrinsic White‐Light Emission via Strongly Localized 1D Excitonic Recombination