1. Effect of Core/Shell Interface on Carrier Dynamics and Optical Gain Properties of Dual-Color Emitting CdSe/CdS Nanocrystals
- Author
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Pinchetti, V, Meinardi, F, Camellini, A, Sirigu, G, Christodoulou, S, Bae, W, De Donato, F, Manna, L, Zavelani Rossi, M, Moreels, I, Klimov, V, Brovelli, S, PINCHETTI, VALERIO, MEINARDI, FRANCESCO, BROVELLI, SERGIO, Pinchetti, V, Meinardi, F, Camellini, A, Sirigu, G, Christodoulou, S, Bae, W, De Donato, F, Manna, L, Zavelani Rossi, M, Moreels, I, Klimov, V, Brovelli, S, PINCHETTI, VALERIO, MEINARDI, FRANCESCO, and BROVELLI, SERGIO
- Abstract
Two-color emitting colloidal semiconductor nanocrystals (NCs) are of interest for applications in multimodal imaging, sensing, lighting, and integrated photonics. Dual color emission from core- and shell-related optical transitions has been recently obtained using so-called dot-in-bulk (DiB) CdSe/CdS NCs comprising a quantum-confined CdSe core embedded into an ultrathick (∼7-9 nm) CdS shell. The physical mechanism underlying this behavior is still under debate. While a large shell volume appears to be a necessary condition for dual emission, comparison between various types of thick-shell CdSe/CdS NCs indicates a critical role of the interface "sharpness" and the presence of potential barriers. To elucidate the effect of the interface morphology on the dual emission, we perform side-by-side studies of CdSe/CdS DiB-NCs with nominally identical core and shell dimensions but different structural properties of the core/shell interface arising from the crystal structure of the starting CdSe cores (zincblende vs wurtzite). While both structures exhibit dual emission under comparable pump intensities, NCs with a zincblende core show a faster growth of shell luminescence with excitation fluence and a more readily realized regime of amplified spontaneous emission (ASE) even under "slow" nanosecond excitation. These distinctions can be linked to the structure of the core/shell interface: NCs grown from the zincblende cores contain a ∼3.5 nm thick zincblende CdS interlayer, which separates the core from the wurtzite CdS shell and creates a potential barrier for photoexcited shell holes inhibiting their relaxation into the core. This helps maintain a higher population of shell states and simplifies the realization of dual emission and ASE involving shell-based optical transitions.
- Published
- 2016