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Plankian Calculator Does Not Match Pr655 Light Readings

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Abstract

Lighting accounts for one-fifth of global electricity consumption1. Single materials with efficient and stable white-lite emission are platonic for lighting applications, but photon emission covering the unabridged visible spectrum is difficult to achieve using a single material. Metallic halide perovskites have outstanding emission propertiestwo,3; all the same, the all-time-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn–Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into CstwoAgInCl6, we break the night transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductoriv. This leads to an increase in photoluminescence efficiency past three orders of magnitude compared to pure CstwoAgInCl6. The optimally alloyed Cs2(Ag0.lxNa0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white lite with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-calorie-free-emitting phosphors and diodes for next-generation lighting and display technologies.

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The datasets analysed during the study are available from the corresponding authors upon request.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51761145048 and 61725401), the National Cardinal R&D Program of China (2016YFB0700702, 2016YFA0204000 and 2016YFB0201204), the HUST Key Innovation Squad for Interdisciplinary Promotion (2016JCTD111) and the Program for JLU Science and Technology Innovative Enquiry Team. The adding of broadband emission at the University of Toledo was supported by the Center for Hybrid Organic Inorganic Semiconductors for Free energy (CHOISE), an Energy Frontier Research Center funded by the Role of Bones Energy Sciences, Role of Science within the US Department of Energy. The analysis of the electronic properties of halide double perovskites was funded past the Part of Free energy Efficiency and Renewable Energy (EERE), U.s.a. Department of Energy, under award number DE-EE0006712. Part of the lawmaking evolution was supported past the National Science Foundation under contract number DMR-1807818. Y.Y. acknowledges support from the Ohio Research Scholar Program. For the theoretical calculations we used the resources of the National Free energy Research Scientific Computing Center, which is supported by the Office of Scientific discipline of the US Section of Energy under contract number DE-AC02-05CH11231. Y.Grand. and J.E. acknowledge financial support by the Australian Research Council (DP150104483) and the use of instrumentation at the Monash Centre for Electron Microscopy. The authors from HUST thank the Analytical and Testing Center of HUST and the facility back up of the Centre for Nanoscale Characterization and Devices, WNLO. We also thank Z. Xiao for useful discussion about emission mechanisms and some XRD measurements, likewise as T. Zhai, H. Vocal, Y. Zhou, H. Han, X. Lu and L. Xu for providing access to some facilities.

Reviewer information

Nature thanks C. C. Stoumpos and the other anonymous reviewer(due south) for their contribution to the peer review of this work.

Author information

Author notes

  1. These authors contributed equally: Jiajun Luo, Xiaoming Wang, Shunran Li, Jing Liu

Affiliations

  1. Sargent Articulation Research Center, Wuhan National Laboratory for Optoelectronics (WNLO) and School of Optical and Electronic Information, Huazhong University of Science and Technology (HUST), Wuhan, Prc

    Jiajun Luo, Shunran Li, Jing Liu, Guangda Niu, Li Yao, Liang Gao, Meiying Leng, Wenxi Liang & Jiang Tang

  2. Department of Physics and Astronomy and Wright Center for Photovoltaics Innovation and Commercialization, The University of Toledo, Toledo, OH, The states

    Xiaoming Wang & Yanfa Yan

  3. Department of Materials Scientific discipline and Engineering, Monash University, Clayton, Victoria, Commonwealth of australia

    Yueming Guo & Joanne Etheridge

  4. State Key Laboratory of Superhard Materials, Key Laboratory of Automobile Materials of MOE, and School of Materials Science and Technology, Jilin University, Changchun, China

    Yuhao Fu & Lijun Zhang

  5. Section of Electrical and Computer Technology, University of Toronto, Toronto, Ontario, Canada

    Liang Gao & Edward H. Sargent

  6. Primal Laboratory of Organic Optoelectronics and Molecular Engineering of Ministry building of Education, Department of Chemistry, Tsinghua University, Beijing, China

    Qingshun Dong, Fusheng Ma & Liduo Wang

  7. State Key Laboratory of Molecular Reaction Dynamics and Collaborative Innovation Eye of Chemistry for Free energy Materials (iChEM), Dalian Institute of Chemic Physics, Chinese Academy of Sciences, Dalian, China

    Chunyi Zhao & Shengye Jin

  8. Wuhan National Loftier Magnetic Field Center, Huazhong University of Science and Engineering science (HUST), Wuhan, China

    Junbo Han

  9. Monash Centre for Electron Microscopy, Monash Academy, Clayton, Victoria, Australia

    Joanne Etheridge

  10. School of Physics and Technology, Centre for Electron Microscopy, MOE Key Laboratory of Artificial Micro- and Nano-structures, and Establish for Advanced Studies, Wuhan Academy, Wuhan, China

    Jianbo Wang

Contributions

J.T. conceived the idea and guided the whole projection. J. Luo, S.Fifty. and J. Liu designed and performed nearly of the experiments and analysed the data; X.W. performed most of the theoretical calculations and assay (GW-BSE, STE, photoluminescence) under the guidance of Y.Y.; S.Fifty. discovered the phosphor; L.Y. contributed in electroluminescence device optimization; L.G. carried out transient-assimilation experiments; M.L. assisted in data analysis and photoluminescence measurements; Y.G. and J.E. carried out the electron microscopy measurements and analysed the results; Y.F. and 50.Z. faux the band alignment and the contour plots of the valence-ring maximum and conduction-band maximum charge densities; C.Z. and S.J. provided some optical measurements; Q.D., F.M., L.Westward., Westward.L. and J.H. helped in the PLQY measurement and electroluminescence device fabrication; G.Due north. was involved in data analysis and experimental blueprint; J.W. contributed to DFT calculations, Y.Y. helped in manuscript writing; J. Luo, Ten.W., E.H.South. and J.T. wrote the newspaper; all authors commented on the manuscript.

Corresponding authors

Correspondence to Yanfa Yan or Jiang Tang.

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Competing interests

The authors declare no competing interests.

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Publisher's annotation: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Extended data figures and tables

Extended Data Fig. 1 Phonon band construction of CsiiAgInCl6 and the zone-centre Jahn–Teller phonon mode (inset).

The phonon band construction was calculated past the finite-divergence method with the supercell arroyo. The consistency of the displacement pattern of the phonon eigenvector with that of the lattice distortion during STE formation, every bit well as the consistency of the phonon eigenfrequency with the phonon frequency fitted from the configuration coordinate diagram, confirm that the Jahn–Teller phonon style coupled with the photoexcited excitons is responsible for the STE formation in Cs2AgInCl6.

Source information

Extended Data Fig. 2 Emission label of pure CsiiAgInCl6.

a, The wide photoluminescence (PL) spectrum of Cs2AgInClhalf dozen measured at room temperature. b, Temperature-dependent photoluminescence spectra of pure Cs2AgInClhalf dozen. c, Plumbing equipment results of the FWHM every bit a office of temperature. We note that we used a relatively low-temperature region to avert the influence of defect-assisted emission. d, The PLQY of Cs2AgInClsix. The reference was measured in an integrating sphere with a bare quartz plate.

Source data

Extended Information Fig. 3 Electronic and optical properties of CsiiNaInCl6.

a, GW-calculated band structure. The GW bandgap is half-dozen.42 eV. The everyman exciton, with a binding energy of 0.eight eV, is dark. The first bright exciton has a bounden free energy of 0.44 eV. b. Calculated optical absorption ('Abs-theory') and photoluminescence ('PL-theory') spectra are compared with experimental results ('Abs-exp.' and 'PL-exp.').

Source data

Extended Data Fig. four Alloy behaviour of CsiiAg ten Na1−ten InCl6.

a, XRD patterns of CstwoAg x Naane−10 InClsix, shifted to lower degrees with increasing sodium substitution (theta, diffraction angle). b, Refined lattice parameter, plotted as a office of the nominal 10 in Cs2Ag x Na1−10 InCl6, showing a linear increment with increased sodium substitution (see Supplementary Fig. 3 for details of the characterization). We annotation that selected-area electron diffraction and scanning electron nanobeam diffraction analysis results (Supplementary Figs. iv, v) suggest the existence of a microscopic super-lattice (Na/Ag ordering).

Source information

Extended Information Fig. 5 Photoluminescence enhancement of doped double-perovskite powders.

a, Photoluminescence spectra of pure Cs2AgInCl6 and Li-doped Cs2AgInClsix. b, Photoluminescence spectra of pure Cs2AgSbClvi and Na-doped Cs2AgSbClvi.

Source information

Extended Data Fig. 6 Characterization of the effect of Bi doping on Cs2Ag x Na1−10 InClhalf-dozen.

a, High-resolution unmarried-crystal XRD of the (111) peaks of CsiiAg0.60Na0.twoscoreInClvi with and without Bi doping. b, Absorption spectra of various materials with and without Bi doping for wavelengths of 500–950 nm. c, PLQY results. d, Photoluminescence lifetime. e, Comparison of the total density of states (DOS) between pure and Bi-doped Cs2AgInClvi. The inset shows the ring alignment of pure and Bi-doped Cs2AgInClhalf dozen. CBM, conduction ring minimum; VBM, valence ring maximum. The small shallow tiptop marked past an arrow is derived from the Bi 6south states, which hybridize with the Ag 4d states. f, Partial density of states (PDOS) of Bi-doped CstwoAgInCl6.

Source data

Extended Data Table 1 Huang–Rhys factors

Full size tabular array

Supplementary data

Supplementary Information

This file contains the Supplementary Tables (Tables S1–S4) and Supplementary Discussion (Figs. S1–S17) which include: XRD analysis of alloyed CsiiAg x Na1−x InClhalf-dozen powder, inductively coupled plasma optical emission spectrometer (ICP-OES) results of Cs2Ag x Na1−ten InClsix with Bi doping, electron microscopy and diffraction results of a small fraction of Cs2Ag0.60Na0.40InClvi, optical characterization of Cs2Ag 10 Na1−x InClhalf dozen powder, and the pic morphology, device performance and farther improving strategies for thermally evaporated CsiiAg0.60Na0.40InCl6 electroluminescent devices

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Luo, J., Wang, Ten., Li, S. et al. Efficient and stable emission of warm-white light from atomic number 82-complimentary halide double perovskites. Nature 563, 541–545 (2018). https://doi.org/10.1038/s41586-018-0691-0

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  • DOI : https://doi.org/10.1038/s41586-018-0691-0

Keywords

  • Double Perovskite
  • Self-trapped Excitons (STE)
  • Parity-forbidden Transitions
  • Metallic Halide Perovskites
  • Photoluminescence Quantum Yield (PLQY)

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