We report fluorescence blinking statistics measured from single CdSe nanorods (NRs) of seven different sizes with aspect ratios ranging from 3 to 11. This study also included core/shell CdSe/ZnSe NRs and core NRs with two different surface ligands producing different degrees of surface passivation. We compare the findings for NRs to our measurements of blinking statistics from spherical CdSe core and CdSe/ZnS core/shell nanocrystals (NCs). We find that, for both NRs and spherical NCs, the off-time probability distributions are well described by a power law, while the on-time probability distributions are best described by a truncated power law, P(tau(on)) approximately tau(on)(-alpha)e((-tau)(on)/(tau)(c)). The measured crossover time, tau(c), is indistinguishable within experimental uncertainty for core and core/shell NRs, as well as for core NRs with different ligands, for the same core size, indicating that surface passivation does not affect the blinking statistics significantly. We find that, at fixed excitation intensity, 1/tau(c) increases approximately linearly with increasing NR aspect ratio; for a given sample, 1/tau(c) increases very gradually with increasing excitation intensity. Examining 1/tau(c)versus the single-particle photon absorption rate for all samples indicates that the change in NR absorption cross section with sample size can account for some but not all of the differences in crossover time. This suggests that the degree of quantum confinement may be partially responsible for the aspect ratio dependence of the crossover time.
We report measurements of the excitation energy dependence of the fluorescence intermittency of single CdSe/ZnS core/shell nanocrystals (NCs), using two different sizes of NCs and three different excitation energies. The lowest excitation energy corresponds to exciting the smaller size NC at its optical band gap, so we examine both excitation at the band gap and at varying energies above the band gap. We find that off-time probability distributions follow a power law with exponent roughly -1.5 regardless of NC size or excitation energy. The on-time probability distributions follow a truncated power law with a power-law exponent that again does not depend on size or energy. With comparable absorption rate, the truncation times for the larger nanocrystals are very similar when excited either 270 or 480 meV above the band gap but shorten for nearultraviolet excitation 1 eV above the band gap. For the smaller nanocrystals, the truncation times are comparable whether excited at the band gap or 270 meV above. Our findings support a spectral diffusion-controlled model for blinking and are consistent with the existence of a quasicontinuous manifold of excited states with altered emission dynamics above the 1P e state; they also indicate a change in emission dynamics at very high excess energy.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.