Search for: All records

Colloidal nanocrystals consist of an inorganic crystalline core with organic ligands bound to the surface and naturally self-assemble into periodic arrays known as superlattices. This periodic structure makes superlattices promising for phononic crystal applications. To explore this potential, we use plane wave expansion methods to model the phonon band structure. We find that the nanoscale periodicity of these superlattices yield phononic band gaps with very high center frequencies on the order of 10 2 GHz. We also find that the large acoustic contrast between the hard nanocrystal cores and the soft ligand matrix lead to very large phononic band gap widths on the order of 10 1 GHz. We systematically vary nanocrystal core diameter, d , nanocrystal core elastic modulus, E NC core , interparticle distance ( i.e. ligand length), L , and ligand elastic modulus, E ligand , and report on the corresponding effects on the phonon band structure. Our modeling shows that the band gap center frequency increases as d and L are decreased, or as E NC core and E ligand are increased. The band gap width behaves non-monotonically with d , L , E NC core , and E ligand , and intercoupling of these variables can eliminate the band gap. Lastly, we observe multiple phononic band gaps in many superlattices and find a correlation between an increase in the number of band gaps and increases in d and E NC core . We find that increases in the property mismatch between phononic crystal components ( i.e. d / L and E NC core / E ligand ) flattens the phonon branches and are a key driver in increasing the number of phononic band gaps. Our predicted phononic band gap center frequencies and widths far exceed those in current experimental demonstrations of 3-dimensional phononic crystals. This suggests that colloidal nanocrystal superlattices are promising candidates for use in high frequency phononic crystal applications. 

The use of nanoparticle-in-matrix composites is a common motif among a broad range of nanoscience applications and is of particular interest to the thermal sciences community. To explore this morphological theme, we create crystalline inorganic composites with nanoparticle volume fractions ranging from 0 to ∼100% using solution-phase processing. We synthesize these composites by mixing colloidal CdSe nanocrystals and In 2 Se 3 metal–chalcogenide complex (MCC) precursor in the solution-phase and then thermally transform the MCC precursor into a crystalline In 2 Se 3 matrix. We find rich structural and chemical interactions between the CdSe nanocrystals and the In 2 Se 3 matrix, including alterations in In 2 Se 3 grain size and orientation as well as the formation of a ternary phase, CdIn 2 Se 4 . The average thermal conductivities of the 100% In 2 Se 3 and ∼100% CdSe composites are 0.32 and 0.53 W m −1 K −1 , respectively. These thermal conductivities are remarkably low for inorganic crystalline materials and are comparable to amorphous polymers. With the exception of the ∼100% CdSe samples, the thermal conductivities of these nanocomposites are insensitive to CdSe volume fraction and are ∼0.3 W m −1 K −1 in all cases. We attribute this insensitivity to competing effects that arise from structural morphology changes during composite formation. This insensitivity to CdSe volume fraction also suggests that very low thermal conductivities can be reliably achieved using this solution-phase route to nanocomposites.