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Weak Exciton–Phonon Coupling in CdSe Nanoplatelets from Quantitative Resonance Raman Intensity Analysis

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journal contribution
posted on 08.11.2018, 00:00 by Cassandra J. A. Maddux, David F. Kelley, Anne Myers Kelley
Resonance Raman spectra, cross sections, and depolarization ratios have been measured for 4.5 monolayer thick CdSe nanoplatelets dispersed in chloroform. Five excitation wavelengths between 514.5 and 476.5 nm were employed. The resonance Raman spectra are dominated by the longitudinal optical (LO) phonon near 201 cm–1 and its overtone, as in CdSe quantum dots. The absolute scattering intensity is much higher for excitation on resonance with the sharp, lowest-energy heavy-hole to conduction band transition than with higher energy transitions, decreasing by about a factor of 30 between 514.5 and 496.5 nm excitation. The LO phonon overtone is weak directly on resonance with the heavy-hole transition but much stronger at higher excitation energies, a result that is reproduced by simulations of the spectra using standard resonance Raman intensity theory. The absolute Raman cross sections imply a Huang–Rhys parameter for the LO phonon of about 0.08 on resonance with the lowest heavy-hole transition. This is a factor of 2–3 lower than found previously for CdSe quantum dots. The depolarization ratios on resonance with the lowest heavy-hole excitonic transition are slightly higher than expected for a degenerate, plane-polarized transition even when the local field factors are taken into account.