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Ilaria Zardo

Publications and source records attributed to Ilaria Zardo.

21 records · Page 2Linked to original sources

Experimental demonstration of the suppression of optical phonon splitting in 2D materials by Raman spectroscopy

Raman spectroscopy is one of the most extended experimental techniques to investigate thin-layered 2D materials. For a complete understanding and modeling of the Raman spectrum of a novel 2D material, it is often necessary to combine the experimental investigation to density-functional-theory calculations. We provide the experimental proof of the fundamentally different behavior of polar 2D vs 3D systems regarding the effect of the dipole-dipole interactions, which in 2D systems ultimately lead to the absence of optical phonons splitting, otherwise present in 3D materials. We demonstrate that non-analytical corrections (NACs) should not be applied to properly model the Raman spectra of few-layered 2D materials, such as WSe$_{2}$ and h-BN, corroborating recent theoretical predictions [Nano Lett. 2017, 17 (6), 3758-3763]. Our findings are supported by measurements performed on tilted samples that allow increasing the component of photon momenta in the plane of the flake, thus unambiguously setting the direction of an eventual NAC. We also investigate the influence of the parity of the number of layers and of the type of layer-by-layer stacking on the effect of NACs on the Raman spectra.

cond-mat.mtrl-sci↗

New insights in the lattice dynamics of monolayers, bilayers, and trilayers of WSe2 and unambiguous determination of few-layer-flakes' thickness

Among the most common few-layers transition metal dichalcogenides (TMDs), WSe2 is the most challenging material from the lattice dynamics point of view. Indeed, for a long time the main two phonon modes (A1g and E12g) have been wrongly assigned. In the last few years, these two modes have been properly interpreted, and their quasi-degeneracy in the monolayer has been used for its identification. In this work, we show that this approach has a limited validity and we propose an alternative, more general approach, based on multi-phonon bands. Moreover, we show and interpret all the peaks (about 40) appearing in the Raman spectra of monolayers, bilayers, and trilayers of WSe2 by combining experimental wavelength- and polarization-dependent Raman studies with density-functional theory calculations providing the phonon dispersions, the polarization-resolved first-order Raman spectra, and the one- and two-phonon density of states. This complete study not only offers a method to distinguish between monolayers, bilayers, and trilayers with no need of optical images and atomic force microscopy, but it also sheds light on the interpretation of single and multi-phonon bands appearing in the inelastic light scattering experiments of layered WSe2; some of these bands were never observed before, and some were observed and uncertainly assigned. We promote the full understanding of the lattice dynamics of this material that is crucial for the realization of optoelectronics devices and of novel phononic metamaterials, such as TMDs superlattices.

cond-mat.mtrl-sci↗

Effects of Dielectric Stoichiometry on the Photoluminescence Properties of Encapsulated WSe2 Monolayers

Two-dimensional transition-metal-dichalcogenide semiconductors have emerged as promising candidates for optoelectronic devices with unprecedented properties and ultra-compact performances. However atomically thin materials are highly sensitive to surrounding dielectric media, which imposes severe limitations to their practical applicability. Hence for their suitable integration into devices, the development of reliable encapsulation procedures that preserve their physical properties are required. Here, the excitonic photoluminescence of WSe2 monolayer flakes is assessed, at room temperature and 10 K, on mechanically exfoliated flakes encapsulated with SiOx and AlxOy layers employing chemical and physical deposition techniques. Conformal flakes coating on untreated - non-functionalized - flakes is successfully demonstrated by all the techniques except for atomic layer deposition, where a cluster-like oxide coating is observed. No significant compositional or strain state changes in the flakes are detected upon encapsulation by any of the techniques. Remarkably, our results evidence that the flakes' optical emission is strongly influenced by the quality of the encapsulating oxide - stoichiometry -. When the encapsulation is carried out with slightly sub-stoichiometric oxides two remarkable phenomena are observed. First, there is a clear electrical doping of the monolayers that is revealed through a dominant trion - charged exciton - room-temperature photoluminescence. Second, a strong decrease of the monolayers optical emission is measured attributed to non-radiative recombination processes and/or carriers transfer from the flake to the oxide. Power- and temperature-dependent photoluminescence measurements further confirm that stoichiometric oxides obtained by physical deposition lead to a successful encapsulation.

cond-mat.mes-hall↗