No Arabic abstract
Positron annihilation lifetime spectroscopy (PALS) and positron-electron momentum density (PEMD) studies on multilayers of PbSe nanocrystals (NCs), supported by transmission electron microscopy (TEM), show that positrons are strongly trapped at NC surfaces, where they provide insight into the surface composition and electronic structure of PbSe NCs. Our analysis indicates abundant annihilation of positrons with Se electrons at the NC surfaces and with O electrons of the oleic ligands bound to Pb ad-atoms at the NC surfaces, which demonstrates that positrons can be used as a sensitive probe to investigate the surface physics and chemistry of nanocrystals inside multilayers. Ab-initio electronic structure calculations provide detailed insight in the valence and semi-core electron contributions to the positron-electron momentum density of PbSe. Both lifetime and PEMD are found to correlate with changes in the particle morphology characteristic of partial ligand removal.
The effect of temperature controlled annealing on the confined valence electron states in CdSe nanocrystal arrays, deposited as thin films, was studied using two-dimensional angular correlation of annihilation radiation (2D-ACAR). A reduction in the intensity by ~35% was observed in a feature of the positron annihilation spectrum upon removal of the pyridine capping molecules above 200 degrees Celsius in a vacuum. This reduction is explained by an increased electronic interaction of the valence orbitals of neighboring nanocrystals, induced by the formation of inorganic interfaces. Partial evaporation of the nanoporous CdSe layer and additional sintering into a polycrystalline thin film was observed at a relatively low temperature of ~486 degrees Celsius.
Nanoscale 3D surface modifications, by scanning tunneling microscopy under ambient conditions, of La0.7Sr0.3MnO3 thin films have been performed. It was demonstrated that there are well defined combinations of bias voltages and scan speeds which allow for controlled surface structuring. Lateral structures with sizes down to 1.5 nm are possible to obtain. Moreover, it is possible to reproducibly control the depth of etching with half a unit cell precision, enabling design of 3D surface structures and control of the surface termination of La0.7Sr0.3MnO3 through etching.
We report electrical transport measurements of arrays of PbSe nanocrystals forming the channels of field effect transistors. We measure the current in these devices as a function of source-drain voltage, gate voltage and temperature. Annealing is necessary to observe measurable current after which a simple model of hopping between intrinsic localized states describes the transport properties of the nanocrystal solid. We find that the majority carriers are holes, which are thermally released from acceptor states. At low source-drain voltages, the activation energy for the conductivity is given by the energy required to generate holes plus the activation over barriers resulting from site disorder. At high source-drain voltages the activation energy is given by the former only. The thermal activation energy of the zero-bias conductance indicates that the Fermi energy is close to the highest-occupied valence level, the 1Sh state, and this is confirmed by field-effect measurements, which give a density of states of approximately eight per nanocrystal as expected from the degeneracy of the 1Sh state.
We demonstrate terahertz time-domain spectroscopy (THz-TDS) to be an accurate, rapid and scalable method to probe the interaction-induced Fermi velocity renormalization { u}F^* of charge carriers in graphene. This allows the quantitative extraction of all electrical parameters (DC conductivity {sigma}DC, carrier density n, and carrier mobility {mu}) of large-scale graphene films placed on arbitrary substrates via THz-TDS. Particularly relevant are substrates with low relative permittivity (< 5) such as polymeric films, where notable renormalization effects are observed even at relatively large carrier densities (> 10^12 cm-2, Fermi level > 0.1 eV). From an application point of view, the ability to rapidly and non-destructively quantify and map the electrical ({sigma}DC, n, {mu}) and electronic ({ u}F^* ) properties of large-scale graphene on generic substrates is key to utilize this material in applications such as metrology, flexible electronics as well as to monitor graphene transfers using polymers as handling layers.
Transitions metal dichalcogenides (TMDs) are direct semiconductors in the atomic monolayer (ML) limit with fascinating optical and spin-valley properties. The strong optical absorption of up to 20 % for a single ML is governed by excitons, electron-hole pairs bound by Coulomb attraction. Excited exciton states in MoSe$_2$ and MoTe$_2$ monolayers have so far been elusive due to their low oscillator strength and strong inhomogeneous broadening. Here we show that encapsulation in hexagonal boron nitride results in emission line width of the A:1$s$ exciton below 1.5 meV and 3 meV in our MoSe$_2$ and MoTe$_2$ monolayer samples, respectively. This allows us to investigate the excited exciton states by photoluminescence upconversion spectroscopy for both monolayer materials. The excitation laser is tuned into resonance with the A:1$s$ transition and we observe emission of excited exciton states up to 200 meV above the laser energy. We demonstrate bias control of the efficiency of this non-linear optical process. At the origin of upconversion our model calculations suggest an exciton-exciton (Auger) scattering mechanism specific to TMD MLs involving an excited conduction band thus generating high energy excitons with small wave-vectors. The optical transitions are further investigated by white light reflectivity, photoluminescence excitation and resonant Raman scattering confirming their origin as excited excitonic states in monolayer thin semiconductors.