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Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in InGaP quantum dots.

作者信息

Li Beiye C, Lin Kailai, Wu Ping-Jui E, Gupta Aritrajit, Peng Kaiyue, Sohoni Siddhartha, Ondry Justin C, Zhou Zirui, Bellora Caitlin C, Ryu Young Jay, Chariton Stella, Gosztola David J, Prakapenka Vitali B, Schaller Richard D, Talapin Dmitri V, Rabani Eran, Engel Gregory S

机构信息

Department of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of Chicago, Chicago, IL, USA.

Institute for Biophysical Dynamics, The University of Chicago, Chicago, IL, USA.

出版信息

Nat Commun. 2025 May 13;16(1):4424. doi: 10.1038/s41467-025-58800-8.


DOI:10.1038/s41467-025-58800-8
PMID:40360464
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12075781/
Abstract

Quantum dots leverage quantum confinement to modify the electronic structure of materials, separating electronic transitions from the composition of the corresponding bulk material. With ternary quantum dots, the composition may be varied continuously so that both composition and size may be used to tune the bandgap. As composition influences electron-phonon coupling which in turn governs relaxation dynamics, the composition of ternary quantum dots may be adjusted to change dynamics. Here, we show that exciton-phonon coupling and phonon-assisted exciton relaxation dynamics remain strongly correlated to material composition in ternary InGaP/ZnS and InGaP/ZnS quantum dots using both experimental two-dimensional electronic spectroscopy measurements and quantum dynamical simulations. Theoretical calculations show that alloyed InGaP quantum dots have more complex exciton level structure than parent InP quantum dots. We identify a slower hot exciton cooling rate in InGaP/ZnS, attributed to the presence of 'energy-retaining' valley exciton states with strong exciton-phonon coupling. Experimental quantum beating maps reveal a more localized quantum beat pattern for InGaP/ZnS quantum dots, which may relate to the increased number of 'dim' exciton levels with reduced spacings. These findings highlight that exciton relaxation dynamics and exciton-phonon coupling in an alloyed InGaP quantum dot system are composition-dependent.

摘要
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/f8b816b9fb91/41467_2025_58800_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/17268bcbe915/41467_2025_58800_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/0c5789df9086/41467_2025_58800_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/8ce37407aaf4/41467_2025_58800_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/f8b816b9fb91/41467_2025_58800_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/17268bcbe915/41467_2025_58800_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/0c5789df9086/41467_2025_58800_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/8ce37407aaf4/41467_2025_58800_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/393e/12075781/f8b816b9fb91/41467_2025_58800_Fig4_HTML.jpg

相似文献

[1]
Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in InGaP quantum dots.

Nat Commun. 2025-5-13

[2]
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[3]
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[4]
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[5]
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[6]
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[7]
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[8]
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[9]
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[10]
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本文引用的文献

[1]
Intrinsically Slow Cooling of Hot Electrons in CdSe Nanocrystals Compared to CdS.

Nano Lett. 2025-1-8

[2]
Reductive pathways in molten inorganic salts enable colloidal synthesis of III-V semiconductor nanocrystals.

Science. 2024-10-25

[3]
Two-Dimensional Electronic Spectroscopy Reveals Dynamics within the Bright Fine Structure of CdSe Quantum Dots.

J Phys Chem Lett. 2024-2-15

[4]
Polaritonic Bottleneck in Colloidal Quantum Dots.

Nano Lett. 2023-11-22

[5]
Theory of Photoluminescence Spectral Line Shapes of Semiconductor Nanocrystals.

J Phys Chem Lett. 2023-8-17

[6]
Composition-Defined Optical Properties and the Direct-to-Indirect Transition in Core-Shell InGaP/ZnS Colloidal Quantum Dots.

J Am Chem Soc. 2023-8-2

[7]
Highly stable and pure single-photon emission with 250 ps optical coherence times in InP colloidal quantum dots.

Nat Nanotechnol. 2023-9

[8]
Exciton Dephasing by Phonon-Induced Scattering between Bright Exciton States in InP/ZnSe Colloidal Quantum Dots.

ACS Nano. 2023-7-11

[9]
Incoherent nonadiabatic to coherent adiabatic transition of electron transfer in colloidal quantum dot molecules.

Nat Commun. 2023-5-27

[10]
Narrow Intrinsic Line Widths and Electron-Phonon Coupling of InP Colloidal Quantum Dots.

ACS Nano. 2023-2-28

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