Temperature-independent emission in a [(CH3)3NPh]2MnBr4 single crystal analogous to thermally activated delayed fluorescence
Source abstract
Abstract
We demonstrate a novel defect-mediated, thermally-activated emission mechanism in [(CH3)3NPh]2MnBr4 single crystals, driven by the coexistence of temperature-sensitive shallow traps and temperature-independent deep traps introduced by Br vacancies. Through comprehensive temperature-dependent photoluminescence (PL) and time-resolved PL measurements, combined with first-principles calculations, we reveal that the material exhibits exceptional thermal stability, retaining 67 % of its relative PL quantum yield at room temperature and achieving an absolute quantum yield of ∼38.9 % under optimal excitation conditions. The dual-component PL decay dynamics consist of a fast decay (∼hundreds of ps) governed by shallow traps and a long decay (∼350 μs) dominated by deep traps, creating an energy cascade that efficiently promotes radiative recombination while minimizing non-radiative losses. Our findings provide critical insights into defect-mediated, thermally-sensitive delayed emission mechanisms and establish [(CH3)3NPh]2MnBr4 as a lead-free, thermally stable material with high efficiency, making it an excellent candidate for next-generation optoelectronic applications, including solid-state lighting and temperature-sensitive devices.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Perovskite Materials and Applications · Organic and Molecular Conductors Research · Luminescence and Fluorescent Materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (51)
Show source-provided references
1. Reverse intersystem crossing from upper triplet levels to excited singlet: a “hot excition” path for organic light-emitting diodes10.1098/rsta.2014.0318 ↗
2. Metal-halide perovskites for photovoltaic and light-emitting devices10.1038/nnano.2015.90 ↗
3. Properties and potential optoelectronic applications of lead halide perovskite nanocrystals10.1126/science.aam7093 ↗
4. Perovskite photonic sources10.1038/nphoton.2016.62 ↗
5. Low-temperature solution-processed wavelength-tunable perovskites for lasing10.1038/nmat3911 ↗
6. Dynamic ultralong phosphorescence and optical waveguiding switches in silver-organic complex via reversible single-crystal-to-single-crystal conversion10.1002/anie.202502782 ↗
7. Solid-State photochemical cascade process boosting smart ultralong room-temperature phosphorescence in bismuth halides10.1002/anie.202402634 ↗
8. Dynamic photoresponsive ultralong phosphorescence from one-dimensional halide microrods toward multilevel information storage10.31635/ccschem.023.202202605 ↗
9. Unlocking full-spectrum brilliance: dimensional regulation in lead-free metal halides for superior photoluminescence10.1021/acs.nanolett.4c03843 ↗
10. Double perovskite Cs2AgInCl6:cr3+: broadband and near-infrared luminescent materials10.1039/C9QI00905A ↗
11. Revealing the nature of photoluminescence emission in the metal-halide double perovskite Cs2AgBiBr610.1039/C9TC02402F ↗
12. Highly efficient phosphorescent emission from organic electroluminescent devices10.1038/25954 ↗
13. Nearly 100% internal phosphorescence efficiency in an organic light-emitting device10.1063/1.1409582 ↗
14. Triplet–triplet annihilation based upconversion- from triplet sensitizers and triplet acceptors to upconversion quantum yields10.1039/c1ra00469g ↗
15. Ultralow-loss optical waveguides through balancing deep-blue TADF and orange room temperature phosphorescence in hybrid antimony halide microstructures10.1002/anie.202309913 ↗
16. Full-color, time-valve controllable and Janus-type long-persistent luminescence from all-inorganic halide perovskites10.1038/s41467-024-49654-7 ↗
17. Upconversion and multiexciton generation in organic Mn(ii) complex boost the quantum yield to >100%10.1039/D2QM00447J ↗
18. Improving the light-harvesting of amorphous silicon solar cells with photochemical upconversion10.1039/c2ee21136j ↗
19. Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites10.1038/s41467-019-08326-7 ↗
20. Efficient charge generation by relaxed charge-transfer states at organic interfaces koen10.1038/nmat3807 ↗
21. Electron-phonon coupling in hybrid lead halide perovskites10.1038/ncomms11755 ↗
22. Charge-carrier dynamics in organic-inorganic metal halide perovskites10.1146/annurev-physchem-040215-112222 ↗
23. Origin of unusual bandgap shift and dual emission in organic-inorganic lead halide perovskites10.1126/sciadv.1601156 ↗
24. Simultaneous long-persistent blue luminescence and high quantum yield within 2D organic–Metal halide perovskite micro/nanosheets10.1002/anie.201909760 ↗
25. Efficient thermally activated delayed fluorescence from all-inorganic cesium zirconium halide perovskite nanocrystals10.1002/anie.202009101 ↗
26. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set10.1103/PhysRevB.54.11169 ↗
27. Generalized gradient approximation made simple10.1103/PhysRevLett.77.3865 ↗
28. Accurate molecular van der Waals interactions from ground-state electron density and free-atom reference data10.1103/PhysRevLett.102.073005 ↗
29. High photoluminescence quantum yield in band gap tunable bromide containing mixed halide perovskites10.1021/acs.nanolett.5b04884 ↗
30. Excitation-power dependence ofthe near-band-edge photoluminescence of semiconductors10.1103/PhysRevB.45.8989 ↗
31. Equal footing of thermal expansion and electron−phonon interaction in the temperature dependence of lead halide perovskite band gaps10.1021/acs.jpclett.9b00876 ↗
32. Intrinsic white-light emission from layered hybrid perovskites10.1021/ja507086b ↗
33. Structural phase transition causing anomalous photoluminescence behavior in perovskite (C6H11NH3)2[PbI4]10.1063/1.4936776 ↗
34. Formation of long-lived color centers for broadband visible light emission in low-dimensional layered perovskites10.1021/jacs.7b10223 ↗
35. Broadband extrinsic self-trapped exciton emission in Sn-doped 2D lead-halide perovskites10.1002/adma.201806385 ↗
36. Temperature-dependent photoluminescence of PbS quantum dots in glass: evidence of exciton state splitting and carrier trapping10.1103/PhysRevB.82.125320 ↗
37. Direct–indirect character of the bandgap inmethylammounium lead iodide perovskite10.1038/nmat4765 ↗
38. Defects in perovskite-halides and their effects in solar cells10.1038/nenergy.2016.149 ↗
39. Giant bandgap renormalization and exciton–phononScattering in perovskite nanocrystals10.1002/adom.201700231 ↗
40. Multi-excitonic complexes in single InGaN quantum dots10.1063/1.1751214 ↗
41. Luminescence linewidths of excitons in GaAs quantum wells below 150 K10.1103/PhysRevB.33.5512 ↗
42. High-efficiency luminescence and robust thermal quenching resistance in organic–Inorganic hybrid indium-based metal halides10.1002/adom.202402409 ↗
43. High photoluminescence efficiency and optically pumped lasing in solution-processed mixed halide perovskite semiconductors10.1021/jz5005285 ↗
44. Interpreting time-resolved photoluminescence of perovskite materials10.1039/D0CP04950F ↗
45. Temperature-dependent photoluminescence spectra and decay dynamics of MAPbBr3 and MAPbI3 thin films
46. Exciton localization in solution-processed organolead trihalide perovskites10.1038/ncomms10896 ↗
47. Long-lived dark exciton emission in Mn-doped CsPbCl3 perovskite nanocrystals10.1021/acs.jpcc.8b12035 ↗
48. Electron‑hole excitations and optical spectra from first principles10.1103/PhysRevB.62.4927 ↗
49. Anharmonicity-driven Rashba cohelical excitons break quantum efficiency limitation10.1002/adma.202005400 ↗
50. Electron‑energy‑loss spectra and the structural stability of nickel oxide: an LSDA+ U study10.1103/PhysRevB.57.1505 ↗
51. Impacts of carrier capture processes in the thermal quenching of photoluminescence in Al–N co-doped SiC10.1007/s00340-019-7279-8 ↗