Slower Auger Recombination in 12-Faceted Dodecahedron CsPbBr Nanocrystals

Overview

Journal J Phys Chem Lett

Publisher American Chemical Society

Specialty Chemistry

Date 2023 Jan 25

PMID 36696665

Authors

Supriya Ghosh

Bapi Pradhan

Weihua Lin

Yiyue Zhang

Luca Leoncino

Pavel Chabera

Kaibo Zheng

Eduardo Solano

Johan Hofkens

Tonu Pullerits

Affiliations

Soon will be listed here.

Abstract

Over the past two decades, intensive research efforts have been devoted to suppressions of Auger recombination in metal-chalcogenide and perovskite nanocrystals (PNCs) for the application of photovoltaics and light emitting devices (LEDs). Here, we have explored dodecahedron cesium lead bromide perovskite nanocrystals (DNCs), which show slower Auger recombination time compared to hexahedron nanocrystals (HNCs). We investigate many-body interactions that are manifested under high excitation flux density in both NCs using ultrafast spectroscopic pump-probe measurements. We demonstrate that the Auger recombination rate due to multiexciton recombinations are lower in DNCs than in HNCs. At low and intermediate excitation density, the majority of carriers recombine through biexcitonic recombination. However, at high excitation density (>10 cm) a higher number of many-body Auger process dominates over biexcitonic recombination. Compared to HNCs, high PLQY and slower Auger recombinations in DNCs are likely to be significant for the fabrication of highly efficient perovskite-based photonics and LEDs.

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References

Trinh M, Sfeir M, Choi J, Owen J, Zhu X . A hot electron-hole pair breaks the symmetry of a semiconductor quantum dot. Nano Lett. 2013; 13(12):6091-7. DOI: 10.1021/nl403368y. View

Protesescu L, Yakunin S, Bodnarchuk M, Krieg F, Caputo R, Hendon C . Nanocrystals of Cesium Lead Halide Perovskites (CsPbX₃, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut. Nano Lett. 2015; 15(6):3692-6. PMC: 4462997. DOI: 10.1021/nl5048779. View

Nedelcu G, Protesescu L, Yakunin S, Bodnarchuk M, Grotevent M, Kovalenko M . Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, I). Nano Lett. 2015; 15(8):5635-40. PMC: 4538456. DOI: 10.1021/acs.nanolett.5b02404. View

Yan F, Tan S, Li X, Demir H . Light Generation in Lead Halide Perovskite Nanocrystals: LEDs, Color Converters, Lasers, and Other Applications. Small. 2019; 15(47):e1902079. DOI: 10.1002/smll.201902079. View

Cappel U, Feldt S, Schoneboom J, Hagfeldt A, Boschloo G . The influence of local electric fields on photoinduced absorption in dye-sensitized solar cells. J Am Chem Soc. 2010; 132(26):9096-101. DOI: 10.1021/ja102334h. View

Ghosh S, Shi Q, Pradhan B, Kumar P, Wang Z, Acharya S . Phonon Coupling with Excitons and Free Carriers in Formamidinium Lead Bromide Perovskite Nanocrystals. J Phys Chem Lett. 2018; 9(15):4245-4250. DOI: 10.1021/acs.jpclett.8b01729. View

Valkunas L, Akesson E, Pullerits T, Sundstrom V . Energy migration in the light-harvesting antenna of the photosynthetic bacterium Rhodospirillum rubrum studied by time-resolved excitation annihilation at 77 K. Biophys J. 1996; 70(5):2373-9. PMC: 1225213. DOI: 10.1016/S0006-3495(96)79804-1. View

Bublitz G, Boxer S . Stark spectroscopy: applications in chemistry, biology, and materials science. Annu Rev Phys Chem. 1997; 48:213-42. DOI: 10.1146/annurev.physchem.48.1.213. View

Jiang Y, Cui M, Li S, Sun C, Huang Y, Wei J . Reducing the impact of Auger recombination in quasi-2D perovskite light-emitting diodes. Nat Commun. 2021; 12(1):336. PMC: 7804015. DOI: 10.1038/s41467-020-20555-9. View

10.

Zhang X, Lin H, Huang H, Reckmeier C, Zhang Y, Choy W . Enhancing the Brightness of Cesium Lead Halide Perovskite Nanocrystal Based Green Light-Emitting Devices through the Interface Engineering with Perfluorinated Ionomer. Nano Lett. 2016; 16(2):1415-20. DOI: 10.1021/acs.nanolett.5b04959. View

11.

Roiati V, Mosconi E, Listorti A, Colella S, Gigli G, De Angelis F . Stark effect in perovskite/TiO2 solar cells: evidence of local interfacial order. Nano Lett. 2014; 14(4):2168-74. DOI: 10.1021/nl500544c. View

12.

Kanemitsu Y . Trion dynamics in lead halide perovskite nanocrystals. J Chem Phys. 2019; 151(17):170902. DOI: 10.1063/1.5125628. View

13.

Eperon G, Jedlicka E, Ginger D . Biexciton Auger Recombination Differs in Hybrid and Inorganic Halide Perovskite Quantum Dots. J Phys Chem Lett. 2017; 9(1):104-109. DOI: 10.1021/acs.jpclett.7b02805. View

14.

Hu F, Yin C, Zhang H, Sun C, Yu W, Zhang C . Slow Auger Recombination of Charged Excitons in Nonblinking Perovskite Nanocrystals without Spectral Diffusion. Nano Lett. 2016; 16(10):6425-6430. DOI: 10.1021/acs.nanolett.6b02874. View

15.

Dang Z, Dhanabalan B, Castelli A, Dhall R, Bustillo K, Marchelli D . Temperature-Driven Transformation of CsPbBr Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly. Nano Lett. 2020; 20(3):1808-1818. PMC: 7997623. DOI: 10.1021/acs.nanolett.9b05036. View

16.

Hassan Y, Park J, Crawford M, Sadhanala A, Lee J, Sadighian J . Ligand-engineered bandgap stability in mixed-halide perovskite LEDs. Nature. 2021; 591(7848):72-77. DOI: 10.1038/s41586-021-03217-8. View

17.

Bera S, Behera R, Pradhan N . α-Halo Ketone for Polyhedral Perovskite Nanocrystals: Evolutions, Shape Conversions, Ligand Chemistry, and Self-Assembly. J Am Chem Soc. 2020; 142(49):20865-20874. DOI: 10.1021/jacs.0c10688. View

18.

Wang H, Dou Y, Shen P, Kong L, Yuan H, Luo Y . Molecule-Induced p-Doping in Perovskite Nanocrystals Enables Efficient Color-Saturated Red Light-Emitting Diodes. Small. 2020; 16(20):e2001062. DOI: 10.1002/smll.202001062. View

19.

Bohn B, Tong Y, Gramlich M, Lai M, Doblinger M, Wang K . Boosting Tunable Blue Luminescence of Halide Perovskite Nanoplatelets through Postsynthetic Surface Trap Repair. Nano Lett. 2018; 18(8):5231-5238. DOI: 10.1021/acs.nanolett.8b02190. View

20.

Schlaus A, Spencer M, Miyata K, Liu F, Wang X, Datta I . How lasing happens in CsPbBr perovskite nanowires. Nat Commun. 2019; 10(1):265. PMC: 6335413. DOI: 10.1038/s41467-018-07972-7. View