The application of an electric field through two-dimensional materials (2DMs) modifies their properties. For example, a bandgap opens in semimetallic bilayer graphene while the bandgap shrinks in few-layer 2D semiconductors. The maximum electric field strength achievable in conventional devices is limited to ≤0.3 V/nm by the dielectric breakdown of gate dielectrics. Here, we overcome this limit by suspending a 2DM between two volumes of ionic liquid (IL) with independently controlled potentials. The potential difference between the ILs falls across an ultrathin layer consisting of the 2DM and the electrical double layers above and below it, producing an intense electric field larger than 4 V/nm. This field is strong enough to close the bandgap of few-layer WSe2, thereby driving a semiconductor-to-metal transition. The ability to apply fields an order of magnitude higher than what is possible in dielectric-gated devices grants access to previously-inaccessible phenomena occurring in intense electric fields.
In the field of phononics, periodic patterning controls vibrations and thereby the flow of heat and sound in matter. Bandgaps arising in such phononic crystals (PnCs) realize low-dissipation vibrational modes and enable applications toward mechanical qubits, efficient waveguides, and state-of-the-art sensing. Here, we combine phononics and two-dimensional materials and explore tuning of PnCs via applied mechanical pressure. To this end, we fabricate the thinnest possible PnC from monolayer graphene and simulate its vibrational properties. We find a bandgap in the megahertz regime within which we localize a defect mode with a small effective mass of 0.72 ag = 0.002 mphysical. We exploit graphene’s flexibility and simulate mechanical tuning of a finite size PnC. Under electrostatic pressure up to 30 kPa, we observe an upshift in frequency of the entire phononic system by ∼350%. At the same time, the defect mode stays within the bandgap and remains localized, suggesting a high-quality, dynamically tunable mechanical system.
Interfaces of dye molecules and two-dimensional transition metal dichalcogenides (TMDCs) combine strong molecular dipole excitations with high carrier mobilities in semiconductors. Förster type energy transfer is one key mechanism for the coupling between both constituents. We report microscopic calculations of a spectrally resolved Förster induced transition rate from dye molecules to a TMDC layer. Our approach is based on microscopic Bloch equations which are solved selfconsistently together with Maxwells equations. This approach allows to incorporate the dielectric environment of a TMDC semiconductor, sandwiched between donor molecules and a substrate. Our analysis reveals transfer rates in the meV range for typical dye molecules in closely stacked structures, with a non-trivial dependence of the Förster rate on the molecular transition energy resulting from unique signatures of dark, momentum forbidden TMDC excitons.
The coupled spin and valley degrees of freedom in transition metal dichalcogenides (TMDs) are considered a promising platform for information processing. Here, we use a TMD heterostructure MoS2-MoSe2 to study optical pumping of spin/valley polarized carriers across the interface and to elucidate the mechanisms governing their subsequent relaxation. By applying time-resolved Kerr and reflectivity spectroscopies, we find that the photoexcited carriers conserve their spin for both tunneling directions across the interface. Following this, we measure dramatically different spin/valley depolarization rates for electrons and holes, ~30 ns -1 and <1 ns -1 , respectively and show that this difference relates to the disparity in the spin-orbit splitting in conduction and valence bands of TMDs. Our work provides insights into the spin/valley dynamics of free carriers unaffected by complex excitonic processes and establishes TMD heterostructures as generators of spin currents in spin/valleytronic devices.
Mechanical strain is a powerful tuning knob for excitons, Coulomb-bound electron–hole complexes dominating optical properties of two-dimensional semiconductors. While the strain response of bright free excitons is broadly understood, the behaviour of dark free excitons (long-lived excitations that generally do not couple to light due to spin and momentum conservation) or localized excitons related to defects remains mostly unexplored. Here, we study the strain behaviour of these fragile many-body states on pristine suspended WSe2 kept at cryogenic temperatures. We find that under the application of strain, dark and localized excitons in monolayer WSe2—a prototypical 2D semiconductor—are brought into energetic resonance, forming a new hybrid state that inherits the properties of the constituent species. The characteristics of the hybridized state, including an order-of-magnitude enhanced light/matter coupling, avoided-crossing energy shifts, and strain tunability of many-body interactions, are all supported by first-principles calculations. The hybridized excitons reported here may play a critical role in the operation of single quantum emitters based on WSe2. Furthermore, the techniques we developed may be used to fingerprint unidentified excitonic states.
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