Second harmonic generation in SiC polytypes

LMTO calculations are presented for the frequency dependent second harmonic generation (SHG) in the polytypes 2H, 4H, 6H, 15R and 3C of SiC. All independent tensor components are calculated. The spectral features and the ratios of the 333 to 311 tensorial components are studied as a function of the degree of hexagonality. The relationship to the linear optical response and the underlying band structure are investigated. SHG is suggested to be a sensitive tool for investigating the near band edge interband excitations.Comment: 12 pages, 10 figure

Many-body calculations of plasmon and phonon satellites in angle-resolved photoelectron spectra using the cumulant expansion approach

The interaction of electrons with crystal lattice vibrations (phonons) and collective charge-density fluctuations (plasmons) influences profoundly the spectral properties of solids revealed by photoemission spectroscopy experiments. Photoemission satellites, for instance, are a prototypical example of quantum emergent behavior that may result from the strong coupling of electronic states to plasmons and phonons. The existence of these spectral features has been verified over energy scales spanning several orders of magnitude (from 50 meV to 15-20 eV) and for a broad class of compounds such as simple metals, semiconductors, and highly-doped oxides. During the past few years the cumulant expansion approach, alongside with the GW approximation and the theory of electron-phonon and electron-plasmon coupling in solids, has evolved into a predictive and quantitatively accurate approach for the description of the spectral signatures of electron-boson coupling entirely from first principles, and it has thus become the state-of-the-art theoretical tool for the description of these phenomena. In this chapter we introduce the fundamental concepts needed to interpret plasmon and phonon satellites in photoelectron spectra, and we review recent progress on first-principles calculations of these features using the cumulant expansion method

Nanoscale Visualization of Elastic Inhomogeneities at TiN Coatings Using Ultrasonic Force Microscopy

Ultrasonic force microscopy has been applied to the characterization of titanium nitride coatings deposited by physical vapor deposition dc magnetron sputtering on stainless steel substrates. The titanium nitride layers exhibit a rich variety of elastic contrast in the ultrasonic force microscopy images. Nanoscale inhomogeneities in stiffness on the titanium nitride films have been attributed to softer substoichiometric titanium nitride species and/or trapped subsurface gas. The results show that increasing the sputtering power at the Ti cathode increases the elastic homogeneity of the titanium nitride layers on the nanometer scale. Ultrasonic force microscopy elastic mapping on titanium nitride layers demonstrates the capability of the technique to provide information of high value for the engineering of improved coatings

Performance of hybrid buffer Poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) layers doped with plasmonic silver nanoparticles

We compare the performance of a typical hole transport layer for organic photovoltaics (OPVs), Poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) thin film with a series of PEDOT:PSS layers doped with silver (Ag) nanoparticles (NPs) of various size distributions. These hybrid layers have attracted great attention as buffer layers in plasmonic OPVs, although there is no report up to date on their isolated performance. In the present study we prepared a series of PEDOT:PSS layers sandwiched between indium tin oxide (ITO) and gold (Au) electrodes. Ag NPs were deposited on top of the ITO by electron beam evaporation followed by spin coating of PEDOT:PSS. Electrical characterization performed in the dark showed linear resistive behavior for all the samples; lower resistance was observed for the hybrid ones. It was found that the resistivity of the samples decreases with increasing the particle's size. A substantial increase of the electric field between the ITO and the Au electrodes was seen through the formation of current paths through the Ag NPs. A striking observation is the slight increase in the slope of the current density versus voltage curves when measured under illumination for the case of the plasmonic layers, indicating that changes in the electric field in the vicinity of the NP due to plasmonic excitation is a non-vanishing factor

Development of scalable and versatile nanomaterial libraries for nanosafety studies: polyvinylpyrrolidone (PVP) capped metal oxide nanoparticles

The potential long-term environmental impact of manufactured nanomaterials (NMs) remains poorly understood, and the need to better predict NM fate and transformations and chronic effects is particularly urgent. Compared to their bulk counterparts, manufactured NMs can have distinct physical and chemical characteristics, which influence their behaviour, stability and toxicity. It is therefore essential to develop standard and reference NM libraries for environmental nanoscience and nano(eco)toxicology, and to facilitate a move towards computational prediction of NM fate, through quantitative structure–activity relationships for example. The aim of this work was to develop and fully characterise one such library, which included comparable NMs with a range of core chemistries, but the same capping agent and size range, for use in future studies to test the hypothesis that the core chemistry is a primary factor in controlling toxicity. The library contained the following NMs: 10k, 40k and 360k PVP capped ceria, zinc oxide and copper oxide (9 NMs in total). The work presented here upholds the underpinning hypothesis that the mechanism of NM formation is the same in all cases, suggesting that the protocol is very robust and has the potential to generate a wide range of comparable metal oxide NMs and potentially expand the library further with doped metal oxide and metal NMs. Characterisation by means of DLS (both size and zeta measurements), UV/Vis, XPS, FT-IR, TEM, STEM, EDX and EELS confirms that the tested synthesis protocol can easily and successfully be used to create stable PVP capped metal oxide NMs of reproducible sizes