journal article·2025-01Open access

Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals

Dandan Wang, Yusheng Li, Yongge Yang, Chao Ding, Yuyao Wei, Dong Liu, Hua Li, Huan Bi, Shikai Chen, Sujun Ji, Boyu Zhang, Yao Guo, Huiyun Wei, Hongshi Li, Shuzi Hayase, Qing Shen

eScience· Volume 5· Issue 1

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 ↗