Understanding structure of small TiO2 nanoparticles and adsorption mechanisms of PbS quantum dots for solid-state applications: a combined theoretical and experimental study

• Published in: Theoretical chemistry accounts 2019-07, Vol.138 (7)
• Main Authors: Díaz-Rodríguez, T. G., Pacio, M., Agustín-Serrano, R., Juárez-Santiesteban, Héctor, Muñiz, Jesús
• Format: Article
• Language: English
• Subjects: Atomic/Molecular Structure and Spectra; Chemistry; Chemistry and Materials Science; Inorganic Chemistry; Organic Chemistry; Physical Chemistry; Regular Article; Theoretical and Computational Chemistry
• ISSN: 1432-881X; 1432-2234
• DOI: 10.1007/s00214-019-2480-8

A combined theoretical and experimental study on a series of TiO 2 , lead sulfide (PbS) and PbS@TiO 2 nanocomposites was performed. TiO 2 structures were stabilized with simulated annealing using molecular dynamics at the ReaxFF level. A density functional theory study elucidated relevant electronic structure properties. We performed the study for a series of TiO 2 ) n , where n = 18 , 28, 38, 76 and 114. Band gaps ranging from 1.2 to 2.2 eV were found. This range was attributed to the size of the TiO 2 cluster models used in the calculations, and some models became metallic at smaller sizes. We synthesized TiO 2 nanoparticles of anatase (101) facet, which were characterized with pair distribution functions, in excellent agreement with the theoretical results. We explored the possibility to anchor a PbS quantum dot with a TiO 2 model system. This intermolecular interaction was relevant, since the composite material could be used in solid-state devices' applications, in which stability in the formation of the PbS / TiO 2 interface plays an important role for the device performance. The possibility to form a PbS@TiO 2 composite material was evidenced, via a covalent interaction, with contributions of the van der Waals type.