Single-crystal PbSe nanowires are synthesized in solution through oriented attachment of nanocrystal building blocks. Reaction temperatures of 190-250 degrees C and multicomponent surfactant mixtures result in a nearly defect-free crystal lattice and high uniformity of nanowire diameter along the entire length. The wires' dimensions are tuned by tailoring reaction conditions in a range from approximately 4 to approximately 20 nm in diameter with wire lengths up to approximately 30 microm. PbSe nanocrystals bind to each other on either {100}, {110}, or {111} faces, depending on the surfactant molecules present in the reaction solution. While PbSe nanocrystals have the centrosymmetric rocksalt lattice, they can lack central symmetry due to a noncentrosymmetric arrangement of Pb- and Se-terminated {111} facets and possess dipole driving one-dimensional oriented attachment of nanocrystals to form nanowires. In addition to straight nanowires, zigzag, helical, branched, and tapered nanowires as well as single-crystal nanorings can be controllably prepared in one-pot reactions by careful adjustment of the reaction conditions.
The relaxation of strongly-confined electrons and holes between 1P and 1S levels in colloidal PbSe nanocrystals has been time-resolved using femtosecond transient absorption spectroscopy. In contrast to II-VI and III-V semiconductor nanocrystals, both electrons and holes are strongly confined in PbSe nanocrystals. Despite the large electron and hole energy level spacings (at least 12 times the optical phonon energy), we consistently observe picosecond time-scale relaxation. Existing theories of carrier relaxation cannot account for these experimental results. Mechanisms that could possibly circumvent the phonon bottleneck in IV-VI quantum dots are discussed.
Layered assembly structures composed of nanomaterials, such as nanocrystals, have attracted considerable attention as promising candidates for new functional devices whose optical, electromagnetic and electronic behaviours are determined by the spatial arrangement of component elements. However, difficulties in handling each constituent layer in a materialspecific manner limit the 3D integration of disparate nanomaterials into the appropriate heterogeneous electronics. Here we report a pick-and-place transfer method that enables the transfer of large-area nanodot assemblies. This solvent-free transfer utilizes a lifting layer and allows for the reliable transfer of a quantum dot (QD) monolayer, enabling layer-by-layer design. With the controlled multistacking of different bandgap QD layers, we are able to probe the interlayer energy transfer among different QD monolayers. By controlling the emission spectrum through such designed monolayer stacking, we have achieved white emission with stable optoelectronic properties, the closest to pure white among the QD lightemitting diodes reported so far.
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