In this letter we present photoluminescence measurements with different excitation energies on single-layer MoS$_2$ and MoSe$_2$ in order to examine the resonance behavior of the conservation of circular polarization in these transition metal dichalc
ogenides. We find that the circular polarization of the emitted light is conserved to 100% in MoS$_2$ and 84% / 79% (A/A$^-$ peaks) in MoSe$_2$ close to resonance. The values for MoSe$_2$ surpass any previously reported value. However, in contrast to previous predictions, the degree of circular polarization decreases clearly at energies less than the two-phonon longitudinal acoustic phonon energy above the resonance. Our findings indicate that at least two competing processes underly the depolarization of the emission in single-layer transition metal dichalcogenides.
Based on emph{ab initio} theoretical calculations of the optical spectra of vertical heterostructures of MoSe$_2$ (or MoS$_2$) and WSe$_2$ sheets, we reveal two spin-orbit-split Rydberg series of excitonic states below the textsl{A} excitons of MoSe$
_2$ and WSe$_2$ with a significant binding energy on the order of 250,meV for the first excitons in the series. At the same time, we predict crystalographically aligned MoSe$_2$/WSe$_2$ heterostructures to exhibit an indirect fundamental band gap. Due to the type-II nature of the MoSe$_2$/WSe$_2$ heterostructure, the indirect transition and the exciton Rydberg series corresponding to a direct transition exhibit a distinct interlayer nature with spatial charge separation of the coupled electrons and holes. The experimentally observed long-lived states in photoluminescence spectra of MoX$_2$/WY$_2$ heterostructure are attributed to such interlayer exciton states. Our calculations further suggest an effect of stacking order on the peak energy of the interlayer excitons and their oscillation strengths.
We report ab initio calculations of the dielectric function of six mono- and bilayer molybdenum dichalcogenides based in a Bethe Salpether equation+G$_0$W$_0$ ansatz, focussing on the excitonic transitions dominating the absorption spectrum up to an
excitation energy of 3,eV. Our calculations suggest that switching chalcogen atoms and the strength of interlayer interactions should affect the detailed composition of the high C peaks in experimental optical spectra of molybdenum dichalcogenides and cause a significant spin-orbit-splitting of the contributing excitonic transitions in monolayer MoSe$_2$ and MoTe$_2$. This can be explained through changes in the electronic dispersion around the Fermi energy along the chalcogen series S$rightarrow$Se$rightarrow$Te that move the van-Hove singularities in the density of states of the two-dimensional materials along the textit{$Gamma$}-textit{K} line in the Brillouin zone. Further, we confirm the distinct interlayer character of the textsl{C} peak transition in few-layer MoS$_2$ that was predicted before from experimental data and show that a similar behaviour can be expected for MoSe$_2$ and MoTe$_2$ as well.
We present a double-resonant Raman mode in few-layer graphene, which is able to probe the number of graphene layers reliably. This so-called N mode on the low-frequency side of the G mode results from a double-resonant Stokes/anti-Stokes process comb
ining a LO and a ZO phonon. Simulations of the double-resonant Raman spectra in bilayer graphene show very good agreement with the experiments. The investigation of the out-of-plane ZO phonon for layer number determination is expected to be transferable to other layered materials like boron nitride.
We report the chemical reaction of single-layer graphene with hydrogen atoms, generated in situ by electron-induced dissociation of hydrogen silsesquioxane (HSQ). Hydrogenation, forming sp3 C-H functionality on the basal plane of graphene, proceeds a
t a higher rate for single than for double layers, demonstrating the enhanced chemical reactivity of single sheet graphene. The net H atom sticking probability on single layers at 300 K is at least 0.03, which exceeds that of double layers by at least a factor of 15. Chemisorbed hydrogen atoms, which give rise to a prominent Raman D band, can be detached by thermal annealing at 100~200 degrees C. The resulting dehydrogenated graphene is activated when photothermally heated it reversibly binds ambient oxygen, leading to hole doping of the graphene. This functionalization of graphene can be exploited to manipulate electronic and charge transport properties of graphene devices.
We report the existence of broad and weakly asymmetric features in the high-energy (G) Raman modes of freely suspended metallic carbon nanotubes of defined chiral index. A significant variation in peak width (from 12 cm-1 to 110 cm-1) is observed as
a function of the nanotubes chiral structure. When the nanotubes are electrostatically gated, the peak widths decrease. The broadness of the Raman features is understood as the consequence of coupling of the phonon to electron-hole pairs, the strength of which varies with the nanotube chiral index and the position of the Fermi energy.
