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Increase of Third-Order Nonlinear Optical Activity of PbS Quantum Dots in Zeolite Y by Increasing Cation Size
journal contribution
posted on 2012-02-08, 00:00 authored by Hyun Sung Kim, Kyung Byung YoonThe third-order nonlinear optical (3NLO) activity of
PbS quantum
dots (QDs) encapsulated in zeolite Y has been expected to depend sensitively
on the countercation of the zeolite host. However, ion exchange of
the pristine countercation, H+, with other cations has
not been possible because the framework decomposes and the QDs aggregate
immediately when the PbS QD-incorporating zeolite Y with H+ as the countercation is exposed to the atmosphere. We now report
that when H+ is transformed to NH4+, the framework of PbS QD-containing zeolite Y does not undergo decomposition
and the PbS QDs do not undergo aggregation to form larger QDs during
the aqueous ion exchange of NH4+ with alkali-metal
ions (MA+ = Li, Na+, K+, Rb+). The 3NLO activity of the MA+-exchanged PbS QD-incorporating zeolite Y film increases with increasing
size of MA+. The stabilization of the surface-bound
exciton by the electron-rich framework oxide and electron-poor cation
is proposed to be responsible for the increase. This is the first
example of a method for systematically increasing the 3NLO activity
of QDs dispersed in a dielectric matrix by systematically changing
its properties. These results will serve as a guideline for future
research and also promote applications of QD-incorporating zeolites
in various fields.