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Amorphous mixed titania-tantala coatings are key components of Bragg reflectors in the gravitational wave detectors (GWDs). Attaining the lowest possible values of optical absorption and mechanical losses in the coatings is of paramount importance for GWDs, and this requires a complex optimization of the coating deposition and post-deposition annealing. We present here a systematic investigation of the optical properties and internal friction of amorphous mixed titania-tantala coatings grown by ion beam sputtering. We consider coatings with six different cation mixing ratios and we study them both in the as-deposited and annealed state. By exploiting spectroscopic ellipsometry data and modelling, along with ancillary techniques, we retrieved the dielectric function of the coatings in a wide spectral range. When varying the mixing ratio and performing the annealing we find monotonic trends for most of the aforementioned properties. Remakably, the post-annealing Urbach energy displays a definite minimum for a mixing ratio around 20%, very close to the composition of the coatings showing the lowest optical absorption for GWDs applications. We suggest that the observed minimum in the Urbach energy depends not only on the mixing ratio, but also on the annealing parameters. On the other hand, the minimum coating loss angle was found to be weakly dependent on the considered measurement frequency and to lie within a rather broad range of Ti content, suggesting that the search for an absolute minimum following post-deposition annealing should be rather sought in the study of the best annealing parameters for each specific cation ratio considered. This work constitutes a reference for the optical properties of the amorphous mixed titania-tantala coatings, and highlights the relevance of the Urbach energy in the optimization process of materials for high-performing Bragg reflectors., Comment: Pre-submission draft

Understanding the interaction between plasmonic nanoparticles and transparent conductive oxides is instrumental to the development of next-generation photovoltaic, opto-electronic and energy-efficient solid-state lighting devices. We investigated the optical response of hybrid media composed of gold nanoparticles deposited on aluminum-doped zinc oxide thin films with varying doping concentration by spectroscopic ellipsometry. The dielectric functions of bare AZO were addressed first, revealing doping-induced effects such as the band-gap shift and the appearance of free carriers. In the hybrid media, a blueshift of the localized surface plasmon resonance of Au NPs as a function of increasing Al-doping of the substrate was observed, ascribed to the occurrence of a charge transfer between the two materials and the doping-dependent variation of the polarizability of the substrate.

The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter systems, and for understanding more deeply the role of hot electrons in technological applications.

The excitation of plasmonic nanoparticles by ultrashort laser pulses sets in motion a complex ultrafast relaxation process involving the gradual re-equilibration of the system's electron gas, lattice and environment. One of the major hurdles in studying these processes is the lack of direct measurements of the dynamic temperature evolution of the system subcomponents. We measured the dynamic optical response of ensembles of plasmonic Au nanoparticles following ultrashort-pulse excitation and we compared it with the corresponding static optical response as a function of the increasing temperature of the thermodynamic bath. Evaluating the two sets of data, the optical fingerprints of equilibrium or off-equilibrium responses could be clearly identified, allowing us to extract a dynamic thermometric calibration scale of the relaxation process, yielding the experimental ultrafast temperature evolution of the plasmonic particles as a function of time.

Transparent Conductive Oxides (TCOs) are a class of materials that combine high optical transparency with high electrical conductivity. This property makes them uniquely appealing as transparent-conductive electrodes in solar cells and interesting for optoelectronics and infrared-plasmonics applications. One of the new challenges that researchers and engineers are facing is merging optical and electrical control in a single device for developing next-generation photovoltaic, opto-electronic devices and energyefficient solid-state lighting. In this work, we investigated the possible variations in the dielectric properties of aluminum-doped ZnO (AZO) upon gating, by means of Spectroscopic Ellipsometry (SE). We investigated the electrical-bias-dependent optical response of thin AZO films fabricated by magnetron sputtering, within a parallel-plane capacitor configuration. We address the possibility to control their optical and electric performances by applying bias, monitoring the effect of charge injection/depletion in the AZO layer by means of in-operando SE vs applied gate voltage.

Monolayer tungsten disulfide ($WS_2$) has recently attracted large interest as a promising material for advanced electronic and optoelectronic devices such as photodetectors, modulators, and sensors. Since these devices can be integrated in a silicon (Si) chip via back-end-of-line (BEOL) processes, the stability of monolayer $WS_2$ in BEOL fabrication conditions should be studied. In this work, the thermal stability of monolayer single-crystal $WS_2$ at typical BEOL conditions is investigated; namely (i) heating temperature of $300$ $^\circ C$, (ii) pressures in the medium- ($10^{-3}$ mbar) and high- ($10^{-8}$ mbar) vacuum range; (iii) heating times from $30$ minutes to $20$ hours. Structural, optical and chemical analyses of $WS_2$ are performed via scanning electron microscopy (SEM), Raman spectroscopy, photoluminescence (PL) and X-ray photoelectron spectroscopy (XPS). It is found that monolayer single-crystal $WS_2$ is intrinsically stable at these temperature and pressures, even after $20$ hours of thermal treatment. The thermal stability of $WS_2$ is also preserved after exposure to low-current electron beam ($12$ pA) or low-fluence laser ($0.9$ $mJ/\mu m^2$), while higher laser fluencies cause photo-activated degradation upon thermal treatment. These results are instrumental to define fabrication and in-line monitoring procedures that allow the integration of $WS_2$ in device fabrication flows without compromising the material quality., Comment: 21 pages, 5 figures

We report on the results of an extensive campaign of optical and mechanical characterization of the ion-beam sputtered oxide layers (Ta$_2$O$_5$, TiO$_2$, Ta$_2$O$_5$-TiO$_2$, SiO$_2$) within the high-reflection coatings of the Advanced LIGO, Advanced Virgo and KAGRA gravitational-wave detectors: refractive index, thickness, optical absorption, composition, density, internal friction and elastic constants have been measured; the impact of deposition rate and post-deposition annealing on coating internal friction has been assessed. For Ta$_2$O$_5$ and SiO$_2$ layers, coating internal friction increases with the deposition rate, whereas the annealing treatment either erases or largely reduces the gap between samples with different deposition history. For Ta$_2$O$_5$-TiO$_2$ layers, the reduction of internal friction due to TiO$_2$ doping becomes effective only if coupled with annealing. All measured samples showed a weak dependence of internal friction on frequency ($\phi_c(f) = af^{b}$, with $-0.208 < b < 0.140$ depending on the coating material considered). SiO$_2$ films showed a mode-dependent loss branching, likely due to spurious losses at the coated edge of the samples. The reference loss values of the Advanced LIGO and Advanced Virgo input (ITM) and end (ETM) mirror HR coatings have been updated by using our estimated value of Young's modulus of Ta$_2$O$_5$-TiO$_2$ layers (120 GPa) and are about 10\% higher than previous estimations.

We have investigated by spectroscopic ellipsometry (SE, 190-1700 nm) the optical properties of uniform, amorphous thin films of Ta2O5 and Nb2O5 as deposited and after annealing, and after so-called "doping" with Ti atoms which leads to mixed oxides. Ta2O5 and Ti:Ta2O5 are currently used as high-index components in Bragg reflectors for Gravitational Wave Detectors. Parallel to the optical investigation, we measured the mechanical energy dissipation of the same coatings, through the so-called "loss angle" phi = Q^-1, which quantifies the energy loss in materials. By applying the well-known Cody-Lorentz model in the analysis of SE data we have been able to derive accurate information on the fundamental absorption edge through important parameters related to the electronic density of states, such as the optical gap (E_g) and the energy width of the exponential Urbach tail (the Urbach energy E_U). We have found that E_U is neatly reduced by suitable annealing as is also perceptible from direct inspection of SE data. Ti-doping also points to a minor decrease of E_U. The reduction of E_U parallels a lowering of the mechanical losses quantified by the loss angle phi. The correlation highlights that both the electronic states responsible of Urbach tail and the internal friction are sensitive to a self-correlation of defects on a medium-range scale, which is promoted by annealing and in our case, to a lesser extent, by doping. These observations may contribute to a better understanding of the relationship between structural and mechanical properties in amorphous oxides.

We report an investigation of the graphene/substrate interface morphology in large-area polycrystalline graphene grown by chemical-vapour deposition and wet-transferred onto Si wafers. We combined spectroscopic ellipsometry, X-ray photoelectron spectroscopy and atomic-force microscopy in order to yield morphological and chemical information about the system. The data showed that wet-transferred samples may randomly exhibit nanosized relief patterns indicative of small water nanopockets trapped between graphene and the underlying substrate. These pockets affect the adhesion of graphene to the substrate, but can be efficiently removed upon a mild annealing in high vacuum. We show that ellipsometry is capable of successfully and reliably detecting, via multilayer dielectric modelling, both the presence of such a spurious intercalation layer and its removal. The fast, broadly applicable and non-invasive character of this technique can therefore promote its application for quickly and reliably assessing the degree of adhesion of graphene transferred onto target substrates, either for ex-post evaluation or in-line process monitoring., Comment: 11 pages, 4 figures

We report on the optical, mechanical and structural characterization of the sputtered coating materials of Advanced LIGO, Advanced Virgo and KAGRA gravitational-waves detectors. We present the latest results of our research program aiming at decreasing coating thermal noise through doping, optimization of deposition parameters and post-deposition annealing. Finally, we propose sputtered Si3N4 as a candidate material for the mirrors of future detectors.

This work reports an electronic and micro-structural study of an appealing system for optoelectronics: tungsten disulphide WS$_2$ on epitaxial graphene (EG) on SiC(0001). The WS$_2$ is grown via chemical vapor deposition (CVD) onto the EG. Low-energy electron diffraction (LEED) measurements assign the zero-degree orientation as the preferential azimuthal alignment for WS$_2$/EG. The valence-band (VB) structure emerging from this alignment is investigated by means of photoelectron spectroscopy measurements, with both high space and energy resolution. We find that the spin-orbit splitting of monolayer WS$_2$ on graphene is of 462 meV, larger than what is reported to date for other substrates. We determine the value of the work function for the WS$_2$/EG to be 4.5$\pm$0.1 eV. A large shift of the WS$_2$ VB maximum is observed as well , due to the lowering of the WS$_2$ work function caused by the donor-like interfacial states of EG. Density functional theory (DFT) calculations carried out on a coincidence supercell confirm the experimental band structure to an excellent degree. X-ray photoemission electron microscopy (XPEEM) measurements performed on single WS$_2$ crystals confirm the van der Waals nature of the interface coupling between the two layers. In virtue of its band alignment and large spin-orbit splitting, this system gains strong appeal for optical spin-injection experiments and opto-spintronic applications in general.

Energy dissipation in amorphous coatings severely affects high-precision optical and quantum transducers. In order to isolate the source of coating loss, we performed an extensive study of Raman scattering and mechanical loss of a thermally-treated sputtered silica coating. Our results show that loss is correlated with the population of three-membered rings of Si-O$_4$ tetrahedral units, and support the evidence that thermal treatment reduces the density of metastable states separated by a characteristic energy of about 0.5 eV, in favour of an increase of the states separated by smaller activation energies. Finally, we conclude that three-fold rings are involved in the relaxation mechanisms only if they belong to more complex chain-like structures of 10 to 100 tetrahedra., Comment: 5 pages, 3 figures

In this work we present a simple pathway to obtain large single-crystal graphene on copper (Cu) foils with high growth rates using a commercially available cold-wall chemical vapour deposition (CVD) reactor. We show that graphene nucleation density is drastically reduced and crystal growth is accelerated when: i) using ex-situ oxidised foils; ii) performing annealing in an inert atmosphere prior to growth; iii) enclosing the foils to lower the precursor impingement flux during growth. Growth rates as high as 14.7 and 17.5 micrometers per minute are obtained on flat and folded foils, respectively. Thus, single-crystal grains with lateral size of about one millimetre can be obtained in just one hour. The samples are characterised by optical microscopy, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy as well as selected area electron diffraction (SAED) and low-energy electron diffraction (LEED), which confirm the high quality and homogeneity of the films. The development of a process for the quick production of large grain graphene in a commonly used commercial CVD reactor is a significant step towards an increased accessibility to millimetre-sized graphene crystals., Comment: Article: 7 pages, 6 figures. Supplementary Information: 5 pages, 7 figures