Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals
Source abstract
Abstract
Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier-phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Perovskite Materials and Applications · Quantum Dots Synthesis And Properties · Optical properties and cooling technologies in crystalline materials
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (39)
Show source-provided references
1. Ultra-bright, efficient and stable perovskite light-emitting diodes10.1038/s41586-022-05304-w ↗
2. Luminescent solar concentrator efficiency enhanced via nearly lossless propagation pathways10.1038/s41566-023-01366-y ↗
3. All-inorganic perovskite nanocrystal scintillators10.1038/s41586-018-0451-1 ↗
4. Controlling the nucleation and growth kinetics of lead halide perovskite quantum dots10.1126/science.abq3616 ↗
5. Biological impact of lead from halide perovskites reveals the risk of introducing a safe threshold10.1038/s41467-019-13910-y ↗
6. The making of a reconfigurable semiconductor with a soft ionic lattice10.1016/j.matt.2021.09.023 ↗
7. Colloidal synthesis of air-stable alloyed CsSn1-xPbxI3 perovskite nanocrystals for use in solar cells10.1021/jacs.7b08628 ↗
8. Stable inorganic colloidal tin and tin–lead perovskite nanocrystals with ultralong carrier lifetime via Sn(IV) control10.1021/jacs.3c10060 ↗
9. Mixed lead-tin halide perovskites for efficient and wavelength-tunable near-infrared light-emitting diodes10.1002/adma.201806105 ↗
10. Bright and stable near-infrared lead-free perovskite light-emitting diodes10.1038/s41566-023-01351-5 ↗
11. Negligible ion migration in tin-based and tin-doped perovskites10.1002/anie.202213932 ↗
12. High-performance CsPb1-xSnxBr3 perovskite quantum dots for light-emitting diodes10.1002/anie.201706860 ↗
13. The significance of polarons and dynamic disorder in halide perovskites10.1021/acsenergylett.1c00506 ↗
14. Regulation of the luminescence mechanism of two-dimensional tin halide perovskites10.1038/s41467-021-27663-0 ↗
15. Unraveling urbach tail effects in high-performance organic photovoltaics: dynamic vs static disorder10.1021/acsenergylett.2c00816 ↗
16. Comparing methods of characterizing energetic disorder in organic solar cells10.1002/aenm.202300329 ↗
17. Dynamic disorder dominates delocalization, transport, and recombination in halide perovskites10.1016/j.chempr.2018.09.001 ↗
18. Trioctylphosphine oxide acts as alkahest for SnX2/PbX2: a general synthetic route to perovskite ASnxPb1-xX3 (A = Cs, FA, MA; X = Cl, Br, I) quantum dots10.1021/acs.chemmater.9b03918 ↗
19. The long-wavelength edge of photographic sensitivity and of the electronic absorption of solids10.1103/PhysRev.92.1324 ↗
20. Optical absorption, charge separation and recombination dynamics in Sn/Pb cocktail perovskite solar cells and their relationships to photovoltaic performances10.1039/C5TA01246E ↗
21. Disorder and the optical-absorption edge of hydrogenated amorphous silicon10.1103/PhysRevLett.47.1480 ↗
22. Light emission from halide perovskite semiconductors: bulk crystals, thin films, and nanocrystals10.1088/1361-6463/ac0e58 ↗
23. Anomalous temperature-dependent exciton–phonon coupling in cesium lead bromide perovskite nanosheets10.1021/acs.jpcc.9b00091 ↗
24. Highly emissive divalent-ion-doped colloidal CsPb1-xMxBr3 perovskite nanocrystals through cation exchange10.1021/jacs.6b13079 ↗
25. The doping mechanism of halide perovskite unveiled by alkaline earth metals10.1021/jacs.9b11637 ↗
26. Temperature dependence of the energy gap in semiconductors10.1016/0031-8914(67)90062-6 ↗
27. Electron-phonon coupling in hybrid lead halide perovskites10.1038/ncomms11755 ↗
28. Effects of the isotopic composition on the fundamental gap of CuCl10.1103/PhysRevB.57.15183 ↗
29. Giant bandgap renormalization and exciton–phonon scattering in perovskite nanocrystals10.1002/adom.201700231 ↗
30. Structural disorder as the origin of optical properties and spectral dynamics in squaraine nano-aggregates10.1021/jacs.2c07064 ↗
31. Lattice strain advances thermoelectrics10.1016/j.joule.2019.02.008 ↗
32. Detection of electron-phonon coupling in two-dimensional materials by light scattering10.1007/s12274-020-2943-1 ↗
33. Low-temperature absorption, photoluminescence, and lifetime of CsPbX3 (X = Cl, Br, I) nanocrystals10.1002/adfm.201800945 ↗
34. Lattice strain causes non-radiative losses in halide perovskites10.1039/C8EE02751J ↗
35. Large polarons in lead halide perovskites10.1126/sciadv.1701217 ↗
36. Quantitative measurement of displacement and strain fields from HREM micrographs10.1016/S0304-3991(98)00035-7 ↗
37. Understanding electron-phonon interactions in 3D lead halide perovskites from the stereochemical expression of 6s(2) lone pairs10.1021/jacs.2c03443 ↗
38. Chemical tuning of dynamic cation off-centering in the cubic phases of hybrid tin and lead halide perovskites10.1039/C7SC01429E ↗
39. First-principles indicators of metallicity and cation off-centricity in the IV-VI rocksalt chalcogenides of divalent Ge, Sn, and Pb10.1103/PhysRevB.67.125111 ↗