Lead Chalcogenide Nanoparticles and Their Size-Controlled Self-Assemblies for Thermoelectric and Photovoltaic Applications
- Caleb K. MiskinCaleb K. MiskinDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Caleb K. Miskin
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- Swapnil D. DeshmukhSwapnil D. DeshmukhDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Swapnil D. Deshmukh
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- Venkata VasirajuVenkata VasirajuDepartment of Chemical Engineering, Texas A&M University, College Station, Texas 77843, United StatesMore by Venkata Vasiraju
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- Kevin BockKevin BockDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Kevin Bock
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- Gaurav MittalGaurav MittalDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Gaurav Mittal
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- Angela Dubois-CamachoAngela Dubois-CamachoDavidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Angela Dubois-Camacho
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- Sreeram VaddirajuSreeram VaddirajuDepartment of Chemical Engineering, Texas A&M University, College Station, Texas 77843, United StatesMore by Sreeram Vaddiraju
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- Rakesh Agrawal*Rakesh Agrawal*E-mail: [email protected]Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United StatesMore by Rakesh Agrawal
Abstract

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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