PbSe Quantum Dot Superlattice Thin Films for Thermoelectric Applications

Author:

Sousa Viviana12ORCID,Goto Masahiro3ORCID,Claro Marcel S.4ORCID,Pyrlin Sergey15ORCID,Marques Luis15,Modin Evgeny B.6ORCID,Lebedev Oleg I.7ORCID,Alizadeh Siavash M.2ORCID,Freitas Cátia2ORCID,Vieira Eliana M. F.89ORCID,Kovnir Kirill1011ORCID,Alpuim Pedro12ORCID,Mori Takao3ORCID,Kolen'ko Yury V.2ORCID

Affiliation:

1. Center of Physics of the Universities of Minho and Porto University of Minho Braga 4710‐057 Portugal

2. International Iberian Nanotechnology Laboratory Braga 4715‐330 Portugal

3. National Institute for Materials Science (NIMS) Research Center for Materials Nanoarchitectonics (MANA) 1‐1 Namiki Tsukuba 305‐0044 Japan

4. CiQUS, Centro Singular de Investigacion en Quimica Bioloxica e Materiais Moleculares Departamento de Quimica‐Fisica Universidade de Santiago de Compostela Santiago de Compostela 15782 Spain

5. Laboratory of Physics for Materials and Emergent Technologies Lap MET University of Minho Braga 4710‐057 Portugal

6. CIC nanoGUNE Donostia San Sebastian 20018 Spain

7. Laboratoire CRISMAT UMR 6508, CNRS‐ENSICAEN Caen 14050 France

8. CMEMS‐UMinho University of Minho Guimarães 4800‐058 Portugal

9. LABBELS‐Associate Laboratory Braga/Guimarães Portugal

10. Department of Chemistry Iowa State University Ames IA 50011 USA

11. U.S. Department of Energy Ames National Laboratory Ames IA 50011 USA

Abstract

AbstractAn unusual self‐assembly pattern is observed for highly ordered 1500‐nm‐thick films of monodisperse 13‐nm‐sized colloidal PbSe quantum dots, originating from their faceted truncated cube‐like shape. Specifically, self‐assembled PbSe dots exhibited attachment to the substrate by <001> planes followed by an interconnection through the {001} facets in plan‐view and {110}/{111} facets in cross‐sectional‐view, thus forming a cubic superlattice. The thermoelectric properties of the PbSe superlattice thin films are investigated by means of frequency domain thermoreflectance, scanning thermal probe microscopy, and four‐probe measurements, and augmented by computational efforts. Thermal conductivity of the superlattice films is measured as low as 0.7 W m−1 K−1 at room temperature due to the developed nanostructure. The low values of electrical conductivity are attributed to the presence of insulating oleate capping ligands at the dots’ surface and the small contact area between the PbSe dots within the superlattice. Experimental efforts aiming at the removal of the oleate ligands are conducted by annealing or molten‐salt treatment, and in the latter case, yielded a promising improvement by two orders of magnitude in thermoelectric performance. The result indicates that the straightforward molten‐salt treatment is an interesting approach to derive thermoelectric dot superlattice thin films over a centimeter‐sized area.

Funder

National Science Foundation

Publisher

Wiley

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