We have measured nonresonant and resonant Raman-scattering spectra from ZnO nanocrystals with an average diameter of 20 nm. Based on our experimental data and comparison with the recently developed theory, we show that the observed shifts of the polar optical-phonon peaks in the resonant Raman spectra are not related to the spatial phonon confinement. The very weak dispersion of the polar optical phonons in ZnO nanocrystals does not lead to any noticeable redshift of the phonon peaks for 20-nm nanocrystals. The observed phonon shifts have been attributed to the local heating effects. We have demonstrated that even the low-power ultraviolet laser excitation, required for the resonant Raman spectroscopy, can lead to the strong local heating of ZnO nanocrystals. The latter causes significant ͑up to 14 cm −1 ͒ redshift of the optical-phonon peaks compared to their position in bulk crystals. Nonresonant Raman excitation does not produce noticeable local heating. The obtained results can be used for identification of the phonons in the Raman spectra of ZnO nanostructures.
The carrier recombination processes in ZnO quantum dots ͑ϳ4 nm in diameter͒, ZnO nanocrystals ͑ϳ20 nm in diameter͒ and bulk ZnO crystal have been studied using photoluminescence ͑PL͒ spectroscopy in the temperature range from 8.5 to 300 K. The obtained experimental data suggest that the ultraviolet PL in ZnO quantum dots originates from recombination of the acceptor-bound excitons for all temperatures. In the larger size ZnO nanocrystals, the recombination of the acceptor-bound excitons is the dominant contribution to PL only at low temperature ͑T Ͻ 150 K͒. For higher temperatures ͑T Ͼ 150 K͒, PL is mostly due to recombination of the donor-bound excitons. Recombination processes in ZnO quantum dots and nanocrystals differ from those in bulk ZnO mainly because of the large surface-to-volume ratio in both types of nanoparticles and, consequently, a large number of acceptor defects near the surface. No strong inhomogeneous broadening has been observed in ultraviolet PL from ZnO quantum dots. Our results shed light on the carrier-recombination processes in ZnO quantum dots and nanocrystals, and can be used for the ZnO nanostructure optimization for the proposed optoelectronic and spintronic applications.
We investigate exciton states theoretically in strained GaN/AlN quantum dots with wurtzite (WZ) and zinc-blende (ZB) crystal structures, as well as strained WZ GaN/AlGaN quantum dots. We show that the strain field significantly modifies the conduction and valence band edges of GaN quantum dots. The piezoelectric field is found to govern excitonic properties of WZ GaN/AlN quantum dots, while it has a smaller effect on WZ GaN/AlGaN, and very little effect on ZB GaN/AlN quantum dots. As a result, the exciton ground state energy in WZ GaN/AlN quantum dots, with heights larger than 3 nm, exhibits a red shift with respect to the bulk WZ GaN energy gap. The radiative decay time of the red-shifted transitions is large and increases almost exponentially from 6.6 ns for quantum dots with height 3 nm to 1100 ns for the quantum dots with height 4.5 nm. In WZ GaN/AlGaN quantum dots, both the radiative decay time and its increase with quantum dot height are smaller than those in WZ GaN/AlN quantum dots. On the other hand, the radiative decay time in ZB GaN/AlN quantum dots is of the order of 0.3 ns, and is almost independent of the quantum dot height. Our results are in good agreement with available experimental data and can be used to optimize GaN quantum dot parameters for proposed optoelectronic applications. I.
Chaotic advection has served as the paradigm for mixing in fluid flows with simple time dependence. Its skeletal structure is based on analysis of invariant attracting and repelling manifolds in fluid flows. Here we develop a finite-time theory for two-dimensional incompressible fluid flows with arbitrary time dependence and introduce a new mixing diagnostic based on it. Besides stretching events around attracting and repelling manifolds, this allows us to detect hyperbolic mixing zones. We used the new diagnostic to forecast the spatial location and timing of oil washing ashore in Plaquemines Parish and Grand Isle, Louisiana, and Pensacola, Florida, in May 2010 and the flow of oil toward Panama City Beach, Florida, in June 2010.
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