Herein, we discuss the features, applications, open challenges and prospects of plasmonics with various classes of two-dimensional semiconductors “beyond graphene”.
We have investigated the electronic response of single crystals of indium selenide by means of angle-resolved photoemission spectroscopy, electron energy loss spectroscopy and density functional theory. The loss spectrum of indium selenide shows the direct free exciton at ~1.3 eV and several other peaks, which do not exhibit dispersion with the momentum. The joint analysis of the experimental band structure and the density of states indicates that spectral features in the loss function are strictly related to single-particle transitions. These excitations cannot be considered as fully coherent plasmons and they are damped even in the optical limit, i.e. for small momenta. The comparison of the calculated symmetry-projected density of states with electron energy loss spectra enables the assignment of the spectral features to transitions between specific electronic states. Furthermore, the effects of ambient gases on the band structure and on the loss function have been probed.
Among the various two-dimensional semiconductors, indium selenide has recently triggered the interest of scientific community, due to its band gap matching the visible region of the electromagnetic spectrum, with subsequent potential applications in optoelectronics and especially in photodetection. In this feature article, we discuss the main issues in the synthesis, the ambient stability and the application capabilities of this novel class of two-dimensional semiconductors, by evidencing open challenges and pitfalls. In particular, we evidence how the growth of single crystals with reduced amount of Se vacancies is crucial in the road map for the exploitation of indium selenide in technology through ambient-stable nanodevices with outstanding values of both mobility of charge carriers and ON/OFF ratio. The surface chemical reactivity of the InSe surface, as well as applications in the fields of broadband photodetection, flexible electronics and solar energy conversion are also discussed.
We explore the broadband excitation spectrum of bulk using electron energy-loss spectroscopy and density-functional theory. In addition to infrared modes related to intraband three-dimensional (3D) Dirac plasmon and interband transitions between the 3D Dirac bands, we observe modes at 3.9, 7.5, and 19.0 eV in the ultraviolet region. The comparison of the excitation spectrum with the calculated orbital-resolved density of states allows us to ascribe spectral features to transitions between specific electronic states. Additionally, we study the thickness dependence of the high-energy-loss peak in the thin films. We show that, unlike graphene, the high-energy EELS peak in thin film gets redshifted by eV with increasing thickness.
Silicene, the two-dimensional allotrope of silicon, is predicted to exist in a low-buckled honeycomb lattice, characterized by semimetallic electronic bands with graphenelike energy-momentum dispersions around the Fermi level (represented by touching Dirac cones). Single layers of silicene are mostly synthesized by depositing silicon on top of silver, where, however, the different phases observed to date are so strongly hybridized with the substrate that not only the Dirac cones, but also the whole valence and conduction states of ideal silicene appear to be lost. Here, we provide evidence that at least part of this semimetallic behavior is preserved by the coexistence of more silicene phases, epitaxially grown on Ag(111). In particular, we combine electron energy loss spectroscopy and time-dependent density functional theory to characterize the low-energy plasmon of a multiphase-silicene/Ag(111) sample, prepared at controlled silicon coverage and growth temperature. We find that this mode survives the interaction with the substrate, being perfectly matched with the -like plasmon of ideal silicene. We therefore suggest that the weakened interaction of multiphase silicene with the substrate may provide a unique platform with the potential to develop different applications based on two-dimensional silicon systems.