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Title: Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

Journal Article · · Chemistry of Materials
 [1];  [2];  [3];  [1];  [2];  [1];  [4]; ORCiD logo [5]; ORCiD logo [6];  [7];  [8];  [9]; ORCiD logo [10]; ORCiD logo [11]
  1. Florida Agricultural and Mechanical Univ. and Florida State Univ. (FAMU-FSU), Tallahassee, FL (United States). College of Engineering, Dept. of Chemical and Biomedical Engineering
  2. Florida State Univ., Tallahassee, FL (United States). Materials Science and Engineering Program
  3. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  4. Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
  5. East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices; East China Normal Univ. (ECNU), Shanghai (China). Dept. of Physics; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  6. East China Normal Univ. (ECNU), Shanghai (China). Key Lab. of Polar Materials and Devices; East China Normal Univ. (ECNU), Shanghai (China). Dept. of Physics
  7. Florida State Univ., Tallahassee, FL (United States). High-Performance Materials Institute (HPMI)
  8. Univ. of Southern California, Los Angeles, CA (United States). Dept. of Chemistry
  9. Florida Agricultural and Mechanical Univ. and Florida State Univ. (FAMU-FSU), Tallahassee, FL (United States). College of Engineering, Dept. of Chemical and Biomedical Engineering; Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
  10. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  11. Florida Agricultural and Mechanical Univ. and Florida State Univ. (FAMU-FSU), Tallahassee, FL (United States). College of Engineering, Dept. of Chemical and Biomedical Engineering; Florida State Univ., Tallahassee, FL (United States). Materials Science and Engineering Program; Florida State Univ., Tallahassee, FL (United States). Dept. of Chemistry and Biochemistry
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Here, we report the synthesis and characterization of (Ph4P)2SbCl5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph4P+) and antimony (Sb3+) chloride salts, (Ph4P)2SbCl5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl52– with strong excited-state structural distortion. Interestingly, (Ph4P)2SbCl5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1435249
Journal Information:
Chemistry of Materials, Vol. 30, Issue 7; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 129 works
Citation information provided by
Web of Science

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Cited By (21)

Hybrid Chloroantimonates(III): Thermally Induced Triple‐Mode Reversible Luminescent Switching and Laser‐Printable Rewritable Luminescent Paper journal June 2019
Microscopic origin of multiple exciton emission in low-dimensional lead halide perovskites journal November 2019
Hybrid Chloroantimonates(III): Thermally Induced Triple‐Mode Reversible Luminescent Switching and Laser‐Printable Rewritable Luminescent Paper journal July 2019
Electronic shell structures, self-trapped excitons, and defect-bound excitons in Li 2 B 12 H 12 journal January 2019
A moisture-stable organosulfonate-based metal–organic framework with intrinsic self-trapped white-light emission journal January 2020
Crystal structure and luminescence properties of lead-free metal halides (C 6 H 5 CH 2 NH 3 ) 3 MBr 6 (M = Bi and Sb) journal January 2020
Optically pumped white light-emitting diodes based on metal halide perovskites and perovskite-related materials journal January 2020
Zero-dimensional metal oxide Li 4 TiO 4 journal January 2019
Enhancing the phosphorescence of hybrid metal halides through molecular sensitization journal January 2019
Organic cation directed hybrid lead halides of zero-dimensional to two-dimensional structures with tunable photoluminescence properties journal January 2019
Lead‐Free Halide Rb 2 CuBr 3 as Sensitive X‐Ray Scintillator journal September 2019
Direct emission from quartet excited states triggered by upconversion phenomena in solid-phase synthesized fluorescent lead-free organic–inorganic hybrid compounds journal January 2019
Colloidal Synthesis and Optical Properties of All‐Inorganic Low‐Dimensional Cesium Copper Halide Nanocrystals journal September 2019
Lead Halide Post‐Perovskite‐Type Chains for High‐Efficiency White‐Light Emission journal February 2019
Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides journal July 2018
Surprising discoveries on the way to an old compound: four transient iodido antimonates journal January 2019
Colloidal Synthesis and Optical Properties of All‐Inorganic Low‐Dimensional Cesium Copper Halide Nanocrystals journal November 2019
Broadband white-light emission from supramolecular piperazinium-based lead halide perovskites linked by hydrogen bonds journal January 2019
Locally collective hydrogen bonding isolates lead octahedra for white emission improvement journal November 2019
Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides journal July 2018
Broadband Emission in Hybrid Organic–Inorganic Halides of Group 12 Metals journal December 2018

Linked Research (1)

Figures / Tables (4)

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