Size and Solvation Effects on Electronic and Optical Properties of PbS Quantum Dots.

PbS quantum dots (QDs), among the most mature nanocrystals obtained by colloidal chemistry, are promising candidates in optoelectronic applications at various operational frequencies. QD device performances are often determined by charge transport, either carrier injection before photoemission or charge detection after photoabsorption, which is significantly influenced by the dielectric environment. Here, we present the electronic structure and the optical gap of PbS QDs versus size for various solvents calculated using ab initio methods including the many-body perturbation approaches. This study highlights the importance of the dielectric environment, pointing out (1) the non-negligible shift of the electronic structure due to the ground state polarization and (2) a substantial impact on the electronic bandgap. The electron-hole binding energy, which varies largely with the QD size and solvent, is well-described by an electrostatic model. This study reveals the fundamental physics of size and solvation effects, which could be useful to design PbS QD-based optoelectronic devices.

The complex optical index of PbS nanocrystal thin films and their use for short wave infrared sensor design.

As nanocrystals (NCs) gain maturity, they become central building blocks for optoelectronics in devices such as solar cells and, more recently, infrared focal plane arrays. Now that the proof of concept of these devices has been established, their optimization requires a deeper understanding of their electronic and optical features to engineer their optoelectronic properties accurately. Though PbS NCs have been extensively investigated, the complex optical index of PbS NC thin films remains mostly unknown. Some previous works have unveiled the optical index for this type of material optimized for solar cells (excitonic peak at 940 nm), but longer wavelengths remain scarce and surface chemistry effects, which are known to be of central importance for layer doping, are simply unexplored. Here, we conduct a systematic investigation of the complex optical index of PbS NC thin films using broadband spectrally resolved ellipsometry. The obtained results are then compared with simulations combining tight-binding (TB) modeling at the NC level and the Bruggeman model to expand the results to the film scale. While TB calculation gives the NC optical indices, we extract the key NC film parameters such as the NC volume fraction and ligand indices by fitting the Bruggeman formula to ellipsometry measurements. We also bring evidence that this joint modeling method can be conducted without the need for ellipsometry data while preserving the main feature of the experimental results. Finally, the unveiled optical indices are used to model the absorption of short-wave infrared diode stacks based on PbS NCs and are relevant for state-of-the-art devices. Our electromagnetic modeling shows that the absorption within the contact is now a major limitation of the current device operated at the telecom wavelength.

Coupling of PZT Thin Films with Bimetallic Strip Heat Engines for Thermal Energy Harvesting.

A thermal energy harvester based on a double transduction mechanism and which converts thermal energy into electrical energy by means of piezoelectric membranes and bimetals, has previously been developed and widely presented in the literature In such a device, the thermo-mechanical conversion is ensured by a bimetal whereas the electro-mechanical conversion is generated by a piezoelectric ceramic. However, it has been shown that only 19% of the mechanical energy delivered by the bimetal during its snap is converted into electrical energy. To extract more energy from the bimetallic strip and to increase the transduction efficiency, a new way to couple piezoelectric materials with bimetals has thus been explored through direct deposition of piezoelectric layers on bimetals. This paper consequently presents an alternative way to harvest heat, based on piezoelectric bimetallic strip heat engines and presents a proof of concept of such a system. In this light, different PZT (Lead zirconate titanate) thin films were synthesized directly on aluminium foils and were attached to the bimetals using conductive epoxy. The fabrication process of each sample is presented herein as well as the experimental tests carried out on the devices. Throughout this study, different thicknesses of the piezoelectric layers and substrates were tested to determine the most powerful configuration. Finally, the study also gives some guidelines for future improvements of piezoelectric bimetals.