Thomas Bielewicz

Highly efficient carrier multiplication in PbS nanosheets

Semiconductor nanocrystals are promising for use in cheap and highly efficient solar cells. A high efficiency can be achieved by carrier multiplication (CM), which yields multiple electron-hole pairs for a single absorbed photon. Lead chalcogenide nanocrystals are of specific interest, since their band gap can be tuned to be optimal to exploit CM in solar cells. Interestingly, for a given photon energy CM is more efficient in bulk PbS and PbSe, which has been attributed to the higher density of states. Unfortunately, these bulk materials are not useful for solar cells due to their low band gap. Here we demonstrate that two-dimensional PbS nanosheets combine the band gap of a confined system with the high CM efficiency of bulk. Interestingly, in thin PbS nanosheets virtually the entire excess photon energy above the CM threshold is used for CM, in contrast to quantum dots, nanorods and bulk lead chalcogenide materials.

Field–effect transistors made of individual colloidal PbS nanosheets

Two-dimensional materials are considered for future quantum devices and are usually produced by extensive methods like molecular beam epitaxy. We report on the fabrication of field–effect transistors using individual ultra-thin lead sulfide nanostructures with lateral dimensions in the micrometer range and a height of a few nanometers as conductive channel produced by a comparatively fast, inexpensive, and scalable colloidal chemistry approach. Contacted with gold electrodes, such devices exhibit p-type behavior and temperature-dependent photoconductivity. Trap states play a crucial role in the conduction mechanism. The performance of the transistors is among the ones of the best devices based on colloidal nanostructures.

Sculpting of Lead Sulfide Nanoparticles by Means of Acetic Acid and Dichloroethane

Abstract Colloidal lead sulfide is a versatile material with great opportunities to tune the bandgap by electronic confinement and to adapt the optical and electrical properties to the target application. We present a new and simple synthetic route to control size and shape of PbS nanoparticles. Increasing concentrations of explicitly added acetic acid are used to tune the shape of PbS nanoparticles from quasi-spherical particles via octahedrons to six-armed stars. The presence of acetate changes the intrinsic surface energies of the different crystal facets and enables the growth along the 〈100〉 direction. Furthermore, the presence of 1,2-dichloroethane alters the reaction kinetics, which results in smaller nanoparticles with a narrower size distribution.

Towards colloidal spintronics through Rashba spin-orbit interaction in lead sulphide nanosheets

Employing the spin degree of freedom of charge carriers offers the possibility to extend the functionality of conventional electronic devices, while colloidal chemistry can be used to synthesize inexpensive and tunable nanomaterials. Here, in order to benefit from both concepts, we investigate Rashba spin–orbit interaction in colloidal lead sulphide nanosheets by electrical measurements on the circular photo-galvanic effect. Lead sulphide nanosheets possess rock salt crystal structure, which is centrosymmetric. The symmetry can be broken by quantum confinement, asymmetric vertical interfaces and a gate electric field leading to Rashba-type band splitting in momentum space at the M points, which results in an unconventional selection mechanism for the excitation of the carriers. The effect, which is supported by simulations of the band structure using density functional theory, can be tuned by the gate electric field and by the thickness of the sheets. Spin-related electrical transport phenomena in colloidal materials open a promising pathway towards future inexpensive spintronic devices.

New ways to synthesize lead sulfide nanosheets-substituted alkanes direct the growth of 2D nanostructures.

Two-dimensional colloidal nanosheets represent very attractive optoelectronic materials. They combine good lateral conductivity with solution-processability and geometry-tunable electronic properties. In the case of PbS nanosheets, so far synthesis has been driven by the addition of chloroalkanes as coligands. Here, we demonstrate how to synthesize two-dimensional lead sulfide nanostructures using other halogen alkanes and primary amines. Further, we show that at a reaction temperature of 170 °C a coligand is not even necessary and the only ligand, oleic acid, controls the anisotropic growth of the two-dimensional structures. Also, using thiourea as a sulfide source, nanosheets with lateral dimensions of over 10 μm are possible.