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Giant-shell CdSe/CdS nanocrystals : exciton coupling to shell phonons investigated by resonant Raman spectroscopy

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Abstract
The interaction between excitons and phonons in semiconductor nanocrystals plays a crucial role in the exciton energy spectrum and dynamics, and thus in their optical properties. We investigate the exciton-phonon coupling in giant-shell CdSe/CdS core-shell nanocrystals via resonant Raman spectroscopy. The Huang-Rhys parameter is evaluated by the intensity ratio of the longitudinal-optical (LO) phonon of CdS with its first multiscattering (2LO) replica. We used four different excitation wavelengths in the range from the onset of the CdS shell absorption to well above the CdS shell band edge to get insight into resonance effects of the CdS LO phonon with high-energy excitonic transitions. The isotropic spherical giant-shell nanocrystals show consistently stronger exciton-phonon coupling as compared to the anisotropic rod-shaped dot-in-rod (DiR) architecture, and the 2LO/L0 intensity ratio decreases for excitation wavelengths approaching the CdS band edge. The strong exciton-phonon coupling in the spherical giant-shell nanocrystals can be related to the delocalization of the electronic wave functions. Furthermore, we observe the radial breathing modes of the GS nanocrystals and their overtones by ultralow frequency Raman spectroscopy with nonresonant excitation, using laser energies well below the band gap of the heteronanocrystals, and highlight the differences between higher-order optical and acoustic phonon modes.
Keywords
SIZE DEPENDENCE, QUANTUM DOTS, HETEROSTRUCTURES, EMISSION, INTERFACE, DYNAMICS, NANORODS, GROWTH

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MLA
Lin, Miao-Ling et al. “Giant-shell CdSe/CdS Nanocrystals : Exciton Coupling to Shell Phonons Investigated by Resonant Raman Spectroscopy.” JOURNAL OF PHYSICAL CHEMISTRY LETTERS 10.3 (2019): 399–405. Print.
APA
Lin, M.-L., Miscuglio, M., Polovitsyn, A., Leng, Y.-C., Martín-García, B., Moreels, I., Tan, P.-H., et al. (2019). Giant-shell CdSe/CdS nanocrystals : exciton coupling to shell phonons investigated by resonant Raman spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 10(3), 399–405.
Chicago author-date
Lin, Miao-Ling, Mario Miscuglio, Anatolii Polovitsyn, Yu-Chen Leng, Beatriz Martín-García, Iwan Moreels, Ping-Heng Tan, and Roman Krahne. 2019. “Giant-shell CdSe/CdS Nanocrystals : Exciton Coupling to Shell Phonons Investigated by Resonant Raman Spectroscopy.” Journal of Physical Chemistry Letters 10 (3): 399–405.
Chicago author-date (all authors)
Lin, Miao-Ling, Mario Miscuglio, Anatolii Polovitsyn, Yu-Chen Leng, Beatriz Martín-García, Iwan Moreels, Ping-Heng Tan, and Roman Krahne. 2019. “Giant-shell CdSe/CdS Nanocrystals : Exciton Coupling to Shell Phonons Investigated by Resonant Raman Spectroscopy.” Journal of Physical Chemistry Letters 10 (3): 399–405.
Vancouver
1.
Lin M-L, Miscuglio M, Polovitsyn A, Leng Y-C, Martín-García B, Moreels I, et al. Giant-shell CdSe/CdS nanocrystals : exciton coupling to shell phonons investigated by resonant Raman spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 2019;10(3):399–405.
IEEE
[1]
M.-L. Lin et al., “Giant-shell CdSe/CdS nanocrystals : exciton coupling to shell phonons investigated by resonant Raman spectroscopy,” JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 10, no. 3, pp. 399–405, 2019.
@article{8607669,
  abstract     = {The interaction between excitons and phonons in semiconductor nanocrystals plays a crucial role in the exciton energy spectrum and dynamics, and thus in their optical properties. We investigate the exciton-phonon coupling in giant-shell CdSe/CdS core-shell nanocrystals via resonant Raman spectroscopy. The Huang-Rhys parameter is evaluated by the intensity ratio of the longitudinal-optical (LO) phonon of CdS with its first multiscattering (2LO) replica. We used four different excitation wavelengths in the range from the onset of the CdS shell absorption to well above the CdS shell band edge to get insight into resonance effects of the CdS LO phonon with high-energy excitonic transitions. The isotropic spherical giant-shell nanocrystals show consistently stronger exciton-phonon coupling as compared to the anisotropic rod-shaped dot-in-rod (DiR) architecture, and the 2LO/L0 intensity ratio decreases for excitation wavelengths approaching the CdS band edge. The strong exciton-phonon coupling in the spherical giant-shell nanocrystals can be related to the delocalization of the electronic wave functions. Furthermore, we observe the radial breathing modes of the GS nanocrystals and their overtones by ultralow frequency Raman spectroscopy with nonresonant excitation, using laser energies well below the band gap of the heteronanocrystals, and highlight the differences between higher-order optical and acoustic phonon modes.},
  author       = {Lin, Miao-Ling and Miscuglio, Mario and Polovitsyn, Anatolii and Leng, Yu-Chen and Martín-García, Beatriz and Moreels, Iwan and Tan, Ping-Heng and Krahne, Roman},
  issn         = {1948-7185},
  journal      = {JOURNAL OF PHYSICAL CHEMISTRY LETTERS},
  keywords     = {SIZE DEPENDENCE,QUANTUM DOTS,HETEROSTRUCTURES,EMISSION,INTERFACE,DYNAMICS,NANORODS,GROWTH},
  language     = {eng},
  number       = {3},
  pages        = {399--405},
  title        = {Giant-shell CdSe/CdS nanocrystals : exciton coupling to shell phonons investigated by resonant Raman spectroscopy},
  url          = {http://dx.doi.org/10.1021/acs.jpclett.8b03211},
  volume       = {10},
  year         = {2019},
}

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