Colloidal nanoplatelets (NPLs) are promising materials
for lasing
applications. The properties are usually discussed in the framework
of 2D materials, where strong excitonic effects dominate the optical
properties near the band edge. At the same time, NPLs have finite
lateral dimensions such that NPLs are not true extended 2D structures.
Here we study the photophysics and gain properties of CdSe/CdS/ZnS
core–shell–shell NPLs upon electrochemical n doping
and optical excitation. Steady-state absorption and PL spectroscopy
show that excitonic effects are weaker in core–shell–shell
nanoplatelets due to the decreased exciton binding energy. Transient
absorption studies reveal a gain threshold of only one excitation
per nanoplatelet. Using electrochemical n doping,
we observe the complete bleaching of the band edge exciton transitions.
Combining electrochemical doping with transient absorption spectroscopy,
we demonstrate that the gain threshold is fully removed over a broad
spectral range and gain coefficients of several thousand cm–1 are obtained. These doped NPLs are the best performing colloidal
nanomaterial gain medium reported to date, with the lowest gain threshold
and broadest gain spectrum and gain coefficients that are 4 times
higher than in n-doped colloidal quantum dots. The low exciton binding
energy due to the CdS and ZnS shells, in combination with the relatively
small lateral size of the NPLs, results in excited states that are
effectively delocalized over the entire platelet. Core–shell
NPLs are thus on the border between strong confinement in QDs and
dominant Coulombic effects in 2D materials. We demonstrate that this
limit is in effect ideal for optical gain and that it results in an
optimal lateral size of the platelets where the gain threshold per
nm2 is minimal.
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