Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots
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 b...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58800-8 |
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| author | Beiye C. Li Kailai Lin Ping-Jui E. Wu Aritrajit Gupta Kaiyue Peng Siddhartha Sohoni Justin C. Ondry Zirui Zhou Caitlin C. Bellora Young Jay Ryu Stella Chariton David J. Gosztola Vitali B. Prakapenka Richard D. Schaller Dmitri V. Talapin Eran Rabani Gregory S. Engel |
| author_facet | Beiye C. Li Kailai Lin Ping-Jui E. Wu Aritrajit Gupta Kaiyue Peng Siddhartha Sohoni Justin C. Ondry Zirui Zhou Caitlin C. Bellora Young Jay Ryu Stella Chariton David J. Gosztola Vitali B. Prakapenka Richard D. Schaller Dmitri V. Talapin Eran Rabani Gregory S. Engel |
| author_sort | Beiye C. Li |
| collection | DOAJ |
| description | 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 In0.62Ga0.38P/ZnS and In0.35Ga0.65P/ZnS quantum dots using both experimental two-dimensional electronic spectroscopy measurements and quantum dynamical simulations. Theoretical calculations show that alloyed In1-xGaxP quantum dots have more complex exciton level structure than parent InP quantum dots. We identify a slower hot exciton cooling rate in In0.62Ga0.38P/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 In0.35Ga0.65P/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 In1-xGaxP quantum dot system are composition-dependent. |
| format | Article |
| id | doaj-art-75415d3ffdf345449c258b0a711e93e4 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-75415d3ffdf345449c258b0a711e93e42025-08-20T03:53:58ZengNature PortfolioNature Communications2041-17232025-05-0116111110.1038/s41467-025-58800-8Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dotsBeiye C. Li0Kailai Lin1Ping-Jui E. Wu2Aritrajit Gupta3Kaiyue Peng4Siddhartha Sohoni5Justin C. Ondry6Zirui Zhou7Caitlin C. Bellora8Young Jay Ryu9Stella Chariton10David J. Gosztola11Vitali B. Prakapenka12Richard D. Schaller13Dmitri V. Talapin14Eran Rabani15Gregory S. Engel16Department of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, University of California, BerkeleyDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, University of California, BerkeleyDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoCenter for Advanced Radiation Sources, The University of ChicagoCenter for Advanced Radiation Sources, The University of ChicagoCenter for Nanoscale Materials, Argonne National LaboratoryCenter for Advanced Radiation Sources, The University of ChicagoCenter for Nanoscale Materials, Argonne National LaboratoryDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoDepartment of Chemistry, University of California, BerkeleyDepartment of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, The University of ChicagoAbstract 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 In0.62Ga0.38P/ZnS and In0.35Ga0.65P/ZnS quantum dots using both experimental two-dimensional electronic spectroscopy measurements and quantum dynamical simulations. Theoretical calculations show that alloyed In1-xGaxP quantum dots have more complex exciton level structure than parent InP quantum dots. We identify a slower hot exciton cooling rate in In0.62Ga0.38P/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 In0.35Ga0.65P/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 In1-xGaxP quantum dot system are composition-dependent.https://doi.org/10.1038/s41467-025-58800-8 |
| spellingShingle | Beiye C. Li Kailai Lin Ping-Jui E. Wu Aritrajit Gupta Kaiyue Peng Siddhartha Sohoni Justin C. Ondry Zirui Zhou Caitlin C. Bellora Young Jay Ryu Stella Chariton David J. Gosztola Vitali B. Prakapenka Richard D. Schaller Dmitri V. Talapin Eran Rabani Gregory S. Engel Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots Nature Communications |
| title | Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots |
| title_full | Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots |
| title_fullStr | Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots |
| title_full_unstemmed | Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots |
| title_short | Exciton-phonon coupling and phonon-assisted exciton relaxation dynamics in In1-xGaxP quantum dots |
| title_sort | exciton phonon coupling and phonon assisted exciton relaxation dynamics in in1 xgaxp quantum dots |
| url | https://doi.org/10.1038/s41467-025-58800-8 |
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