No Arabic abstract
The electrical and thermal behavior of nanoscale devices based on two-dimensional (2D) materials is often limited by their contacts and interfaces. Here we report the temperature-dependent thermal boundary conductance (TBC) of monolayer MoS$_2$ with AlN and SiO$_2$, using Raman thermometry with laser-induced heating. The temperature-dependent optical absorption of the 2D material is crucial in such experiments, which we characterize here for the first time above room temperature. We obtain TBC ~ 15 MWm$^-$$^2$K$^-$$^1$ near room temperature, increasing as ~ T$^0$$^.$$^6$$^5$ in the range 300 - 600 K. The similar TBC of MoS$_2$ with the two substrates indicates that MoS$_2$ is the softer material with weaker phonon irradiance, and the relatively low TBC signifies that such interfaces present a key bottleneck in energy dissipation from 2D devices. Our approach is needed to correctly perform Raman thermometry of 2D materials, and our findings are key for understanding energy coupling at the nanoscale.
The optical susceptibility is a local, minimally-invasive and spin-selective probe of the ground state of a two-dimensional electron gas. We apply this probe to a gated monolayer of MoS$_2$. We demonstrate that the electrons are spin polarized. Of the four available bands, only two are occupied. These two bands have the same spin but different valley quantum numbers. We argue that strong Coulomb interactions are a key aspect of this spontaneous symmetry breaking. The Bohr radius is so small that even electrons located far apart in phase space interact, facilitating exchange couplings to align the spins.
We measure the thermal time constants of suspended single layer molybdenum disulfide drums by their thermomechanical response to a high-frequency modulated laser. From this measurement the thermal diffusivity of single layer MoS$_2$ is found to be 1.14 $times$ 10$^{-5}$ m$^2$/s on average. Using a model for the thermal time constants and a model assuming continuum heat transport, we extract thermal conductivities at room temperature between 10 to 40 W/(m$cdot$K). Significant device-to-device variation in the thermal diffusivity is observed. Based on statistical analysis we conclude that these variations in thermal diffusivity are caused by microscopic defects that have a large impact on phonon scattering, but do not affect the resonance frequency and damping of the membranes lowest eigenmode. By combining the experimental thermal diffusivity with literature values of the thermal conductivity, a method is presented to determine the specific heat of suspended 2D materials, which is estimated to be 255 $pm$ 104 J/(kg$cdot$K) for single layer MoS$_2$.
We report magneto-optical spectroscopy of gated monolayer MoS$_2$ in high magnetic fields up to 28T and obtain new insights on the many-body interaction of neutral and charged excitons with the resident charges of distinct spin and valley texture. For neutral excitons at low electron doping, we observe a nonlinear valley Zeeman shift due to dipolar spin-interactions that depends sensitively on the local carrier concentration. As the Fermi energy increases to dominate over the other relevant energy scales in the system, the magneto-optical response depends on the occupation of the fully spin-polarized Landau levels in both $K/K^{prime}$ valleys. This manifests itself in a many-body state. Our experiments demonstrate that the exciton in monolayer semiconductors is only a single particle boson close to charge neutrality. We find that away from charge neutrality it smoothly transitions into polaronic states with a distinct spin-valley flavour that is defined by the Landau level quantized spin and valley texture.
Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum device technologies. The ability to tailor quantum emission through deterministic defect engineering is of growing importance for realizing scalable quantum architectures. However, a major difficulty is that defects need to be positioned site-selectively within the solid. Here, we overcome this challenge by controllably irradiating single-layer MoS$_{2}$ using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion bombarded MoS$_{2}$ flake with high-quality hBN reveals spectrally narrow emission lines that produce photons at optical wavelengths in an energy window of one to two hundred meV below the neutral 2D exciton of MoS$_{2}$. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the helium ion bombardment. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and exotic Hubbard systems.
The effect of bis(trifluoromethane) sulfonimide (TFSI, superacid) treatment on the optical properties of MoS$_2$ monolayers is investigated by means of photoluminescence, reflectance contrast and Raman scattering spectroscopy employed in a broad temperature range. It is shown that when applied multiple times, the treatment results in progressive quenching of the trion emission/absorption and in the redshift of the neutral exciton emission/absorption associated with both the A and B excitonic resonances. Based on this evolution, a trion complex related to the B exciton in monolayer MoS$_2$ is unambiguously identified. A defect-related emission observed at low temperatures also disappears from the spectrum as a result of the treatment. Our observations are attributed to effective passivation of defects on the MoS$_{2}$ monolayer surface. The passivation reduces the carrier density, which in turn affects the out-of-plane electric field in the sample. The observed tuning of the carrier concentration strongly influences also the Raman scattering in the MoS$_2$ monolayer. An enhancement of Raman scattering at resonant excitation in the vicinity of the A neutral exciton is clearly seen for both the out-of-plane A$_1^{}$ and in-plane E$^{}$ modes. On the contrary, when the excitation is in resonance with a corresponding trion, the Raman scattering features become hardly visible. These results confirm the role of the excitonic charge state plays in the resonance effect of the excitation energy on the Raman scattering in transition metal dichalcogenides.