Journal
ACS APPLIED NANO MATERIALS
Volume 2, Issue 3, Pages 1242-1252Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.8b02125
Keywords
lead chalcogenides; nanoparticles; self-assembly; solution processing; thermoelectrics
Funding
- NSF graduate research fellowship [DGE-0833366]
- NSF [1534691-DMR]
- Texas A&M Institute of Advanced Study via the HEEP Fellowship
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We report a facile, room temperature synthesis of PbS, PbSe, PbSxSe1-x and PbTe nanoparticles and their microscale assemblies by combining a chalcogen solution and a lead halide solution in select thiol-amine mixtures. Selection of an appropriate thiol-amine pair and/or the use of appropriate amine to thiol ratio has demonstrated a size control on nanoparticle self-assemblies ranging from nano- to microscale. Proper washing of these particles has yielded phase-pure and compositionally uniform material with minimal or no presence of any carbonaceous ligands on the particle surface, making it attractive for electronic device fabrication. The resulting PbS material exhibits bandgaps in the range 0.6 eV to as high as 1.2 eV for various assembly sizes. These optical bandgaps confirm the retention of quantum confinement of PbS material even in self-assembled nano/microstructures, which could be an interesting phenomenon for future photovoltaic development. Along with carbon-free, quantum-confined self-assemblies, this chemistry also provides a room temperature and instantaneous reaction route to synthesize individually dispersed PbS and PbSe particles with long chain ligand capping similar to traditional synthesis routes. The PbSe material synthesized from this route shows the ability to alloy with PbS at room temperature in the entire composition range and also demonstrates thermoelectric performance comparable to results in existing undoped PbSe literature.
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