Energy Relaxation and Hot-electron Lifetimes in Single Nanocrystals

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Dardona, Sameh Ibrahim
First, Phillip N.
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Understanding changes in materials properties as a function of size is crucial for both fundamental science development and technological applications. Size restriction results in quantum confinement effects that modify both energy level structures and electron dynamics of solid materials. This study investigates individual quantum states in a single nanocrystal. Single electron charging effects in gold and semiconductor nanocrystals are observed. Charging effects are found to be dominant in samples, where the nanocrystals are weakly coupled to the substrate. For nanocrystals strongly coupled to the substrate, nanocrystal-substrate tunneling rate is larger than tip-nanocrystal tunneling rate. Therefore, the resulting peaks in the dI/dV spectrum are attributed to tunneling through the energy levels of the nanocrystal. A newly developed nanocrystals BEES technique is used successfully to further explore quantized energy levels and electron dynamics in single gold nanocrystals. BEES samples were grown successfully by depositing $unit[10]{nm}$ thick gold on silicon substrates. Nanocrystals are chemically attached to the gold substrate using a self assembled monolayer (SAM) of xyelendithiol molecules. Immobile and single isolated nanocrystals were imaged at low temperature. A BEES turn-on voltage of $unit[0.84]{V}$ was found on nanocrystal-free region of the substrate. The BEES spectrum acquired on a single gold nanocrystal is found to be attenuated by a factor of 10 when compared with BEES acquired on the substrate. The attenuation is attributed to electron relaxation to lower energy states before tunneling out of the nanocrystal. The measured hot electron lifetimes from experimental data were found to be on the order of $unit[16]{picoseconds}$, which is a long time compared to lifetimes in bulk metals or large nanocrystals. The long measured lifetimes result from the molecular-like energy level structures of these small nanocrystals.
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